Jiaxing Huang

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Name: HUANG, JIAXING
Organization: Northwestern University , USA
Department: Department of Materials Science and Engineering
Title: Associate(PhD)

TOPICS

Co-reporter:Xuan Dou;Xingliang He;Andrew R. Koltonow;Qian Wang;Hee Dong Jang;Yip-Wah Chung
PNAS 2016 Volume 113 (Issue 6 ) pp:1528-1533
Publication Date(Web):2016-02-09
DOI:10.1073/pnas.1520994113
Ultrafine particles are often used as lubricant additives because they are capable of entering tribological contacts to reduce friction and protect surfaces from wear. They tend to be more stable than molecular additives under high thermal and mechanical stresses during rubbing. It is highly desirable for these particles to remain well dispersed in oil without relying on molecular ligands. Borrowing from the analogy that pieces of paper that are crumpled do not readily stick to each other (unlike flat sheets), we expect that ultrafine particles resembling miniaturized crumpled paper balls should self-disperse in oil and could act like nanoscale ball bearings to reduce friction and wear. Here we report the use of crumpled graphene balls as a high-performance additive that can significantly improve the lubrication properties of polyalphaolefin base oil. The tribological performance of crumpled graphene balls is only weakly dependent on their concentration in oil and readily exceeds that of other carbon additives such as graphite, reduced graphene oxide, and carbon black. Notably, polyalphaolefin base oil with only 0.01–0.1 wt % of crumpled graphene balls outperforms a fully formulated commercial lubricant in terms of friction and wear reduction.
Co-reporter:Hua-Li Nie; Xuan Dou; Zhihong Tang; Hee Dong Jang
Journal of the American Chemical Society 2015 Volume 137(Issue 33) pp:10683-10688
Publication Date(Web):August 14, 2015
DOI:10.1021/jacs.5b06052
Langmuir–Blodgett (LB) assembly is a classical molecular thin-film processing technique, in which the material is spread onto water surface from a volatile, water-immiscible solvent to create floating monolayers that can be later transferred to solid substrates. LB has also been applied to prepare colloidal thin films with an unparalleled level of microstructural control and thickness, which has enabled the discovery of many exciting collective properties of nanoparticles and the construction of bulk nanostructured materials. To maximize the benefits of LB assembly, the nanoparticles should be well dispersed in both the spreading solvent and on water. This is quite challenging since colloids usually need contrasting surface properties in order to be stable in the water-hating organic solvents and on water surface. In addition, many organic and polymeric nanostructures dissolve in those organic solvents and cannot be processed directly. Using water-liking spreading solvents can avoid this dilemma. However, spreading of water-miscible solvents on water surface is fundamentally challenging due to extensive mixing, which results in significant material loss. Here we report a conceptually simple strategy and a general technique that allows nearly exclusive spreading of such solvents on water surface using electrospray. Since the volume of these aerosolized droplets is reduced by many orders of magnitude, they are readily depleted during the initial spreading step before any significant mixing could occur. The new strategy drastically reduces the burden of material processing prior to assembly and broadens the scope of LB assembly to previously hard-to-process materials. It also avoids the use of toxic volatile organic spreading solvents, improves the reproducibility, and can be readily automated, making LB assembly a more robust tool for colloidal assembly and thin-film fabrication.
Co-reporter:Stanley S. Chou; Yi-Kai Huang; Jaemyung Kim; Bryan Kaehr; Brian M. Foley; Ping Lu; Conner Dykstra; Patrick E. Hopkins; C. Jeffrey Brinker; Jiaxing Huang;Vinayak P. Dravid
Journal of the American Chemical Society 2015 Volume 137(Issue 5) pp:1742-1745
Publication Date(Web):January 22, 2015
DOI:10.1021/ja5107145
Lithiation-exfoliation produces single to few-layered MoS2 and WS2 sheets dispersible in water. However, the process transforms them from the pristine semiconducting 2H phase to a distorted metallic phase. Recovery of the semiconducting properties typically involves heating of the chemically exfoliated sheets at elevated temperatures. Therefore, it has been largely limited to sheets deposited on solid substrates. Here, we report the dispersion of chemically exfoliated MoS2 sheets in high boiling point organic solvents enabled by surface functionalization and the controllable recovery of their semiconducting properties directly in solution. This process connects the scalability of chemical exfoliation with the simplicity of solution processing, ultimately enabling a facile method for tuning the metal to semiconductor transitions of MoS2 and WS2 within a liquid medium.
Co-reporter:Hee Dong Jang, Sun Kyung Kim, Hankwon Chang, Ji-Hyuk Choi, Bong-Gyoo Cho, Eun Hee Jo, Jeong-Woo Choi, Jiaxing Huang
Carbon 2015 Volume 93() pp:869-877
Publication Date(Web):November 2015
DOI:10.1016/j.carbon.2015.06.009
High performance of electrocatalysts for direct methanol fuel cells was demonstrated by three-dimensional (3D) graphene (GR) decorated with platinum (Pt)–gold (Au) alloy nanoparticles (3D-GR/PtAu). The 3D-GR/PtAu composite with a morphology like a crumpled paper ball was synthesized from a colloidal mixture of GR and Pt–Au alloy nanoparticles with aerosol spray drying. The 3D-GR/PtAu had a high specific surface area and electrochemical surface area of up to 238 and 325 m2/g(Pt), respectively, and the electrocatalytic applications of the 3D-GR/PtAu were examined through methanol oxidation reactions. The 3D-GR/PtAu had the highest electrocatalytic activity for methanol oxidation reactions compared with commercial Pt–carbon black and Pt-GR. The 3D-GR/PtAu was also highly sensitive electrocatalytic activity in the methanol oxidation reaction compared with the 2D-GR/Pt–Au. Furthermore, the electrocatalytic activity of the 3D-GR/PtAu had the highest performance among the catalysts containing Pt, Au, and GR for the methanol oxidation reactions. The increased electrocatalytic activity is attributed to the high specific surface area of the 3D formation and the effective surface structure of the Pt–Au alloy nanoparticles.
Co-reporter:Jiayan Luo, Jun Gao, Aoxuan Wang, and Jiaxing Huang
ACS Nano 2015 Volume 9(Issue 10) pp:9432
Publication Date(Web):September 21, 2015
DOI:10.1021/acsnano.5b05259
The family of two-dimensional (2D) materials, in particular MXenes, can now be greatly expanded based on a new “double metal” strategy as reported by Anasori, Xie, and Beidaghi et al. in this issue of ACS Nano. Now that a diverse array of well-defined nanoscale building blocks, especially the 2D systems, has become available, we are better prepared to think about scaling up nanomaterials in the broader context of materials science and engineering. In this Perspective, we construct a roadmap for assembling nanoscale building blocks into bulk nanostructured materials, and define some of the critical challenges and goals. Two-dimensional sheets are uniquely well-suited in this roadmap for constructing dense, bulk-sized samples with scalable material performance or interesting emergent properties.
Co-reporter:Alexer J. Smith;Yung-Huang Chang;Kalyan Raidongia;Tzu-Yin Chen;Lain-Jong Li
Advanced Energy Materials 2014 Volume 4( Issue 14) pp:
Publication Date(Web):
DOI:10.1002/aenm.201400398
Co-reporter:Deepti Krishnan, Kalyan Raidongia, Jiaojing Shao, and Jiaxing Huang
ACS Nano 2014 Volume 8(Issue 1) pp:449
Publication Date(Web):December 3, 2013
DOI:10.1021/nn404805p
Hydrothermal carbonization (HTC) of biomass such as glucose and cellulose typically produces micrometer-sized carbon spheres that are insulating. Adding a very small amount of Graphene oxide (GO) to glucose (e.g., 1:800 weight ratio) can significantly alter the morphology of its HTC product, resulting in more conductive carbon materials with higher degree of carbonization. At low mass loading level of GO, HTC treatment results in dispersed carbon platelets of tens of nanometers in thickness, while at high mass loading levels, free-standing carbon monoliths are obtained. Control experiments with other carbon materials such as graphite, carbon nanotubes, carbon black, and reduced GO show that only GO has significant effect in promoting HTC conversion, likely due to its good water processability, amphiphilicity, and two-dimensional structure that may help to template the initially carbonized materials. GO offers an additional advantage in that its graphene product can act as an in situ heating element to enable further carbonization of the HTC products very rapidly upon microwave irradiation. Similar effect of GO is also observed for the HTC treatment of cellulose.Keywords: biomass; carbon hydrates; carbonization; graphene oxide; hydrothermal; microwave
Co-reporter:Jiayan Luo, Jaemyung Kim, and Jiaxing Huang
Accounts of Chemical Research 2013 Volume 46(Issue 10) pp:2225
Publication Date(Web):February 21, 2013
DOI:10.1021/ar300180n
Graphene-based sheets show promise for a variety of potential applications, and researchers in many scientific disciplines are interested in these materials. Although researchers have developed many ways of generating single atomic layer carbon sheets, chemical exfoliation of graphite powders to graphene oxide (GO) sheets followed by deoxygenation to form chemically modified graphene (CMG) offers a promising route for bulk scale production. The materials processing, which we broadly define as the physical and chemical means to tailor a material’s chemical and microstructures, enables us to control the properties in bulk CMG materials. For example, by processing CMG sheets in different solvents, we can make thin films, blend CMG sheets with other materials, and modify them by chemical reactions. Materials processing methods also allow us to control the interactions between CMG sheets for the assembly of large scale two- or three-dimensional structures with desirable microstructures.This Account highlights a few problems associated with large scale production and processing of GO and CMG. First, we briefly discuss the potential fire risk of GO and CMG when alkaline salt byproducts are not completely removed. These impurities can catalyze carbon combustion. We introduce an improved purification procedure that effectively removes the byproducts and speeds up the production. Next, we address the challenges of imaging GO and CMG sheets on common substrates such as glass and plastics using standard microscopy methods. We have introduced a new technique fluorescence quenching microscopy (FQM), which allows us to observe graphene-based sheets with both high throughput and high contrast on arbitrary substrates and even in solution. Then we focus on how to prevent aggregation in CMG. Aggregation greatly reduces the material processability and accessible surface area, which degrades the material properties. We introduce two strategies to reduce aggregation by (i) reducing the lateral dimension of the sheets to nanometer range to enhance their colloidal stability and (ii) crumpling the sheets into paper ball-like, fractal-dimensional particles to make them aggregation-resistant in both solvents and solid state, even after mechanical compression.Solutions to these material processing challenges can pave the way for further research and development. We hope that the tools and strategies presented in this Account can facilitate the processing and property control of this promising material.
Co-reporter:Stanley S. Chou +; Mrinmoy De +; Jaemyung Kim +; Segi Byun +; Conner Dykstra +; Jin Yu ; Jiaxing Huang +;Vinayak P. Dravid +
Journal of the American Chemical Society 2013 Volume 135(Issue 12) pp:4584-4587
Publication Date(Web):March 11, 2013
DOI:10.1021/ja310929s
MoS2 is a two-dimensional material that is gaining prominence due to its unique electronic and chemical properties. Here, we demonstrate ligand conjugation of chemically exfoliated MoS2 using thiol chemistry. With this method, we modulate the ζ-potential and colloidal stability of MoS2 sheets through ligand designs, thus enabling its usage as a selective artificial protein receptor for β-galactosidase. The facile thiol functionalization route opens the door for surface modifications of solution processable MoS2 sheets.
Co-reporter:Hee Dong Jang, Sun Kyung Kim, Hankwon Chang, Jeong-Woo Choi, Jiaxing Huang
Materials Letters 2013 Volume 106() pp:277-280
Publication Date(Web):1 September 2013
DOI:10.1016/j.matlet.2013.05.033
Co-reporter:Jaemyung Kim, Segi Byun, Alexander J. Smith, Jin Yu, and Jiaxing Huang
The Journal of Physical Chemistry Letters 2013 Volume 4(Issue 8) pp:1227-1232
Publication Date(Web):March 25, 2013
DOI:10.1021/jz400507t
Here, we report that transition-metal dichalcogenides such as MoS2 and WS2 can be decorated with gold nanoparticles by a spontaneous redox reaction with hexachloroauric acid in water. The resulting gold nanoparticles tend to grow at defective sites, and therefore, selective decorations at the edges and the line defects in the basal planes of bulk single crystals were observed. The lithium intercalation–exfoliation process makes the basal planes of chemically exfoliated MoS2 and WS2 sheets much more defective than their single-crystalline counterparts, leading to a more uniform and higher-density deposition of gold nanoparticles. Due to the greatly improved charge transport between adjacent sheets, the resulting MoS2/Au and WS2/Au hybrids show significantly enhanced electrocatalytic performance toward hydrogen evolution reactions.Keywords: 2D nanomaterials; defects; functionalization; nanoparticles; water splitting;
Co-reporter:Jiayan Luo, Hee Dong Jang, and Jiaxing Huang
ACS Nano 2013 Volume 7(Issue 2) pp:1464
Publication Date(Web):January 27, 2013
DOI:10.1021/nn3052378
Graphene is considered a promising ultracapacitor material toward high power and energy density because of its high conductivity and high surface area without pore tortuosity. However, the two-dimensional (2D) sheets tend to aggregate during the electrode fabrication process and align perpendicular to the flow direction of electrons and ions, which can reduce the available surface area and limit the electron and ion transport. This makes it hard to achieve scalable device performance as the loading level of the active material increases. Here, we report a strategy to solve these problems by transforming the 2D graphene sheet into a crumpled paper ball structure. Compared to flat or wrinkled sheets, the crumpled graphene balls can deliver much higher specific capacitance and better rate performance. More importantly, devices made with crumpled graphene balls are significantly less dependent on the electrode mass loading. Performance of graphene-based ultracapacitors can be further enhanced by using flat graphene sheets as the binder for the crumpled graphene balls, thus eliminating the need for less active binder materials.Keywords: aerosol; aggregation; crumpling; graphene; loading level; scalability; ultracapacitor
Co-reporter:Vincent C. Tung, Jen-Hsien Huang, Jaemyung Kim, Alexander J. Smith, Chih-Wei Chu and Jiaxing Huang  
Energy & Environmental Science 2012 vol. 5(Issue 7) pp:7810-7818
Publication Date(Web):11 Apr 2012
DOI:10.1039/C2EE21587J
In this perspective, we describe a new type of photovoltaic all-carbon composites, in which single walled carbon nanotubes (SWCNTs) and fullerenes are directly co-assembled and processed in water using graphene oxide (GO) as a surfactant. Solar cells made with C60/SWCNTs/reduced GO as the active layer and an additional evaporated C60 blocking layer yield a power conversion efficiency of 0.21%, which can be significantly increased to 0.85% by replacing C60 with the better absorber C70. These results suggest the possibility of making a new generation of solution processed all-carbon solar cells, in which all the functional layers are made of graphitic nanomaterials.
Co-reporter:Jaemyung Kim, Laura J. Cote, and Jiaxing Huang
Accounts of Chemical Research 2012 Volume 45(Issue 8) pp:1356
Publication Date(Web):June 4, 2012
DOI:10.1021/ar300047s
Graphite oxide sheets, now called graphene oxide (GO), can be made from chemical exfoliation of graphite by reactions that have been known for 150 years. Because GO is a promising solution-processable precursor for the bulk production of graphene, interest in this old material has resurged. The reactions to produce GO add oxygenated functional groups to the graphene sheets on their basal plane and edges, and this derivatization breaks the π-conjugated network, resulting in electrically insulating but highly water-dispersible sheets.Apart from making graphene, GO itself has many intriguing properties. Like graphene, GO is a two-dimensional (2D) sheet with feature sizes at two abruptly different length scales. The apparent thickness of the functionalized carbon sheet is approximately 1 nm, but the lateral dimensions can range from a few nanometers to hundreds of micrometers. Therefore, researchers can think of GO as either a single molecule or a particle, depending on which length scale is of greater interest. At the same time, GO can be viewed as an unconventional soft material, such as a 2D polymer, highly anisotropic colloid, membrane, liquid crystal, or amphiphile.In this Account, we highlight the soft material characteristics of GO. GO consists of nanographitic patches surrounded by largely disordered, oxygenated domains. Such structural characteristics effectively make GO a 2D amphiphile with a hydrophilic periphery and largely hydrophobic center. This insight has led to better understanding of the solution properties of GO for making thin films and new applications of GO as a surfactant. Changes in pH and sheet size can tune the amphiphilicity of GO, leading to intriguing interfacial activities. In addition, new all-carbon composites made of only graphitic nanostructures using GO as a dispersing agent have potential applications in photovoltaics and energy storage. On the other hand, GO can function as a 2D random diblock copolymer, one block graphitic and the other heavily hydroxylated. Therefore, GO can guide material assembly through π–π stacking and hydrogen bonding. Additionally, the selective etching of the more reactive sp3 blocks produces a porous GO network, which greatly enhances interactions with gas molecules in chemical sensors. With their high aspect ratio, GO colloids can readily align to form liquid crystalline phases at high concentration.As single-atomic, water-dispersible, soft carbon sheets that can be easily converted to a conductive form, this 2D material should continue to inspire many curiosity-driven discoveries and applications at the interfaces of chemistry, materials science, and other disciplines.
Co-reporter:Vincent C. Tung;Jaemyung Kim
Advanced Energy Materials 2012 Volume 2( Issue 3) pp:299-303
Publication Date(Web):
DOI:10.1002/aenm.201100595
Co-reporter:Vincent C. Tung;Jaemyung Kim
Advanced Energy Materials 2012 Volume 2( Issue 3) pp:
Publication Date(Web):
DOI:10.1002/aenm.201290012
Co-reporter:Stanley S. Chou ; Mrinmoy De ; Jiayan Luo ; Vincent M. Rotello ; Jiaxing Huang ;Vinayak. P. Dravid
Journal of the American Chemical Society 2012 Volume 134(Issue 40) pp:16725-16733
Publication Date(Web):September 10, 2012
DOI:10.1021/ja306767y
The role of conventional graphene-oxide in biosensing has been limited to that of a quenching substrate or signal transducer due to size inconsistencies and poor supramolecular response. We overcame these issues by using nanoscale GOs (nGO) as artificial receptors. Unlike conventional GO, nGOs are sheets with near uniform lateral dimension of 20 nm. Due to its nanoscale architecture, its supramolecular response was enhanced, with demonstrated improvements in biomacromolecular affinities. This rendered their surface capable of detecting unknown proteins with cognizance not seen with conventional GOs. Different proteins at 100 and 10 nM concentrations revealed consistent patterns that are quantitatively differentiable by linear discriminant analysis. Identification of 48 unknowns in both concentrations demonstrated a >95% success rate. The 10 nM detection represents a 10-fold improvement over analogous arrays. This demonstrates for the first time that the supramolecular chemistry of GO is highly size dependent and opens the possibility of improvement upon existing GO hybrid materials.
Co-reporter:Kalyan Raidongia
Journal of the American Chemical Society 2012 Volume 134(Issue 40) pp:16528-16531
Publication Date(Web):September 21, 2012
DOI:10.1021/ja308167f
Electrolytes confined in nanochannels with characteristic dimensions comparable to the Debye length show transport behaviors deviating from their bulk counterparts. Fabrication of nanofluidic devices typically relies on expensive lithography techniques or the use of sacrificial templates with sophisticated growth and processing steps. Here we demonstrate an alternative approach where unprecedentedly massive arrays of nanochannels are readily formed by restacking exfoliated sheets of layered materials, such as graphene oxide (GO). Nanochannels between GO sheets are successfully constructed as manifested by surface-charge-governed ion transport for electrolyte concentrations up to 50 mM. Nanofluidic devices based on reconstructed layer materials have distinct advantages such as low cost, facile fabrication, ease of scaling up to support high ionic currents, and flexibility. Given the rich chemical, physical, and mechanical properties of layered materials, they should offer many exciting new opportunities for studying and even manufacturing nanofluidic devices.
Co-reporter:Jiayan Luo, Vincent C. Tung, Andrew R. Koltonow, Hee Dong Jang and Jiaxing Huang  
Journal of Materials Chemistry A 2012 vol. 22(Issue 26) pp:12993-12996
Publication Date(Web):04 May 2012
DOI:10.1039/C2JM30819C
An adhesive and conductive glue was created by synergistic assembly of graphene oxide (GO), single walled carbon nanotubes (SWCNTs) and conjugate polymer PEDOT:PSS in aqueous solution. The GO–SWCNTs–PEDOT:PSS glue can be used as a binder to fabricate metal oxide nanoparticle based ultracapacitors. Since the functional nanoparticles are immersed in this conductive gel, uniform electrical and mechanical interconnect can be achieved, leading to enhanced performance of ultracapacitors.
Co-reporter:Kwonnam Sohn, Yoon Joo Na, Hankwon Chang, Ki-Min Roh, Hee Dong Jang and Jiaxing Huang  
Chemical Communications 2012 vol. 48(Issue 48) pp:5968-5970
Publication Date(Web):17 Apr 2012
DOI:10.1039/C2CC32049E
Oil absorbing graphene capsules are synthesized by capillary molding of graphene oxide (GO) sheets against a polystyrene bead template in evaporating aerosol droplets, followed by simultaneous reduction of GO and decomposition of the polymer template during ultrasonic spray pyrolysis.
Co-reporter:Jiayan Luo, Xin Zhao, Jinsong Wu, Hee Dong Jang, Harold H. Kung, and Jiaxing Huang
The Journal of Physical Chemistry Letters 2012 Volume 3(Issue 13) pp:1824-1829
Publication Date(Web):June 22, 2012
DOI:10.1021/jz3006892
Submicrometer-sized capsules made of Si nanoparticles wrapped by crumpled graphene shells were made by a rapid, one-step capillary-driven assembly route in aerosol droplets. Aqueous dispersion of micrometer-sized graphene oxide (GO) sheets and Si nanoparticles were nebulized to form aerosol droplets, which were passed through a preheated tube furnace. Evaporation-induced capillary force wrapped graphene (a.k.a., reduced GO) sheets around the Si particles, and heavily crumpled the shell. The folds and wrinkles in the crumpled graphene coating can accommodate the volume expansion of Si upon lithiation without fracture, and thus help to protect Si nanoparticles from excessive deposition of the insulating solid electrolyte interphase. Compared to the native Si particles, the composite capsules have greatly improved performance as Li ion battery anodes in terms of capacity, cycling stability, and Coulombic efficiency.Keywords: Coulombic efficiency; crumpled graphene; encapsulation; lithium ion battery; silicon;
Co-reporter:Deepti Krishnan, Franklin Kim, Jiayan Luo, Rodolfo Cruz-Silva, Laura J. Cote, Hee Dong Jang, Jiaxing Huang
Nano Today 2012 Volume 7(Issue 2) pp:137-152
Publication Date(Web):April 2012
DOI:10.1016/j.nantod.2012.02.003
Motivated by both its graphene-oriented applications and its own remarkable properties, interest in graphene oxide (GO) has widely spread across many disciplines. In parallel to the rapid progress of research, industrial-scale production of GO has emerged. GO is highly energetic, thermally unstable and can readily undergo exothermic disproportionation reactions to produce chemically modified graphene under mild heating conditions. This Review highlights the challenges and opportunities associated with GO's thermal instability such as the potential fire risk during large scale production and methods of mitigation, energy efficient way to reduce GO, photothermal patterning and sintering of graphene/polymer composites, and new syntheses using GO as an in situ power source to make nanoparticle decorated graphene composites for energy storage and catalysts.Graphical abstractHighlights► GO is energetic and its exothermic deoxygenation reactions can self-propagate. ► Metal salt by-products can make GO or its graphene product highly flammable. ► Acid-acetone wash can speed up purification of GO by suppressing gelation. ► GO can be photothermally reduced, patterned and welded with polymer. ► GO can be used as an in situ power source to make nanoparticle decorated graphene.
Co-reporter:Jaemyung Kim;Vincent C. Tung
Advanced Energy Materials 2011 Volume 1( Issue 6) pp:
Publication Date(Web):
DOI:10.1002/aenm.201190025
Co-reporter:Jaemyung Kim;Vincent C. Tung
Advanced Energy Materials 2011 Volume 1( Issue 6) pp:1052-1057
Publication Date(Web):
DOI:10.1002/aenm.201100466
Co-reporter:Vincent C. Tung ; Jen-Hsien Huang ; Ian Tevis ; Franklin Kim ; Jaemyung Kim ; Chih-Wei Chu ; Samuel I. Stupp
Journal of the American Chemical Society 2011 Volume 133(Issue 13) pp:4940-4947
Publication Date(Web):March 10, 2011
DOI:10.1021/ja1103734
Heterojunctions between different graphitic nanostructures, including fullerenes, carbon nanotubes and graphene-based sheets, have attracted significant interest for light to electrical energy conversion. Because of their poor solubility, fabrication of such all-carbon nanocomposites typically involves covalently linking the individual constituents or the extensive surface functionalization to improve their solvent processability for mixing. However, such strategies often deteriorate or contaminate the functional carbon surfaces. Here we report that fullerenes, pristine single walled carbon nanotubes, and graphene oxide sheets can be conveniently coassembled in water to yield a stable colloidal dispersion for thin film processing. After thermal reduction of graphene oxide, a solvent-resistant photoconductive hybrid of fullerene−nanotube−graphene was obtained with on−off ratio of nearly 6 orders of magnitude. Photovoltaic devices made with the all-carbon hybrid as the active layer and an additional fullerene block layer showed unprecedented photovoltaic responses among all known all-carbon-based materials with an open circuit voltage of 0.59 V and a power conversion efficiency of 0.21%. The ease of making such surfactant-free, water-processed, carbon thin films could lead to their wide applications in organic optoelectronic devices.
Co-reporter:Vincent C. Tung ; Jaemyung Kim ; Laura J. Cote
Journal of the American Chemical Society 2011 Volume 133(Issue 24) pp:9262-9265
Publication Date(Web):May 26, 2011
DOI:10.1021/ja203464n
Graphene oxide (GO) can be viewed as a two-dimensional, random diblock copolymer with distributed nanosize graphitic patches and highly oxidized domains, thus capable of guiding the assembly of other materials through both π–π stacking and hydrogen bonding. Upon mixing GO and conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) in water, a dispersion with dramatically increased viscosity is obtained, which turns into sticky thin films upon casting. Surprisingly, the insulating GO makes PEDOT much more conductive by altering its chain conformation and morphology. The GO/PEDOT gel can function as a metal-free solder for creating mechanical and electrical connections in organic optoelectronic devices. As a proof-of-concept, polymer tandem solar cells have been fabricated by a direct adhesive lamination process enabled by the sticky GO/PEDOT film. The sticky interconnect can greatly simplify the fabrication of organic tandem architectures, which has been quite challenging via solution processing. Thus, it could facilitate the construction of high-efficiency tandem solar cells with different combinations of solution-processable materials.
Co-reporter:Tae Hee Han ; Yi-Kai Huang ; Alvin T. L. Tan ; Vinayak P. Dravid
Journal of the American Chemical Society 2011 Volume 133(Issue 39) pp:15264-15267
Publication Date(Web):September 6, 2011
DOI:10.1021/ja205693t
Oxidative etching of graphene flakes was observed to initiate from edges and the occasional defect sites in the basal plane, leading to reduced lateral size and a small number of etch pits. In contrast, etching of highly defective graphene oxide and its reduced form resulted in rapid homogeneous fracturing of the sheets into smaller pieces. On the basis of these observations, a slow and more controllable etching route was designed to produce nanoporous reduced graphene oxide sheets by hydrothermal steaming at 200 °C. The degree of etching and the concomitant porosity can be conveniently tuned by etching time. In contrast to nonporous reduced graphene oxide annealed at the same temperature, the steamed nanoporous graphene oxide exhibited nearly 2 orders of magnitude increase in the sensitivity and improved recovery time when used as chemiresistor sensor platform for NO2 detection. The results underscore the efficacy of the highly distributed nanoporous network in the low temperature steam etched GO.
Co-reporter:Ken C. Pradel;Kwonnam Sohn; Jiaxing Huang
Angewandte Chemie 2011 Volume 123( Issue 15) pp:3474-3478
Publication Date(Web):
DOI:10.1002/ange.201100087
Co-reporter:Ken C. Pradel;Kwonnam Sohn; Jiaxing Huang
Angewandte Chemie International Edition 2011 Volume 50( Issue 15) pp:3412-3416
Publication Date(Web):
DOI:10.1002/anie.201100087
Co-reporter:Jiayan Luo, Hee Dong Jang, Tao Sun, Li Xiao, Zhen He, Alexandros P. Katsoulidis, Mercouri G. Kanatzidis, J. Murray Gibson, and Jiaxing Huang
ACS Nano 2011 Volume 5(Issue 11) pp:8943
Publication Date(Web):October 13, 2011
DOI:10.1021/nn203115u
Unlike flat sheets, crumpled paper balls have both high free volume and high compressive strength, and can tightly pack without significantly reducing the area of accessible surface. Such properties would be highly desirable for sheet-like materials such as graphene, since they tend to aggregate in solution and restack in the solid state, making their properties highly dependent on the material processing history. Here we report the synthesis of crumpled graphene balls by capillary compression in rapidly evaporating aerosol droplets. The crumpled particles are stabilized by locally folded, π–π stacked ridges as a result of plastic deformation, and do not unfold or collapse during common processing steps. In addition, they are remarkably aggregation-resistant in either solution or solid state, and remain largely intact and redispersible after chemical treatments, wet processing, annealing, and even pelletizing at high pressure. For example, upon compression at 55 MPa, the regular flat graphene sheets turn into nondispersible chunks with drastically reduced surface area by 84%, while the crumpled graphene particles can still maintain 45% of their original surface area and remain readily dispersible in common solvents. Therefore, crumpled particles could help to standardize graphene-based materials by delivering more stable properties such as high surface area and solution processability regardless of material processing history. This should greatly benefit applications using bulk quantities of graphene, such as in energy storage or conversion devices. As a proof of concept, we demonstrate that microbial fuel electrodes modified by the crumpled particles indeed outperform those modified with their flat counterparts.Keywords: aerosol; aggregation-resistant particles; capillary compression; crumpling; graphene; graphene oxide; strain hardening
Co-reporter:Franklin Kim;Laura J. Cote
Advanced Materials 2010 Volume 22( Issue 17) pp:1954-1958
Publication Date(Web):
DOI:10.1002/adma.200903932

Abstract

Graphene oxide (GO) is a promising precursor for preparing graphene-based composites and electronics applications. Like graphene, GO is essentially one-atom thick but can be as wide as tens of micrometers, resulting in a unique type of material building block, characterized by two very different length scales. Due to this highly anisotropic structure, the collective material properties are highly dependent on how these sheets are assembled. Therefore, understanding and controlling the assembly behavior of GO has become an important subject of research. In this Research News article the surface activity of GO and how it can be employed to create two-dimensional assemblies over large areas is discussed.

Co-reporter:Jaemyung Kim, Franklin Kim, Jiaxing Huang
Materials Today 2010 Volume 13(Issue 3) pp:28-38
Publication Date(Web):March 2010
DOI:10.1016/S1369-7021(10)70031-6
Graphene-based sheets such as graphene, graphene oxide and reduced graphene oxide have stimulated great interest due to their promising electronic, mechanical and thermal properties. Microscopy imaging is indispensable for characterizing these single atomic layers, and oftentimes is the first measure of sample quality. This review provides an overview of current imaging techniques for graphene-based sheets and highlights a recently developed fluorescence quenching microscopy technique that allows high-throughput, high-contrast imaging of graphene-based sheets on arbitrary substrate and even in solution.
Co-reporter:Jaemyung Kim ; Laura J. Cote ; Franklin Kim ; Wa Yuan ; Kenneth R. Shull
Journal of the American Chemical Society 2010 Volume 132(Issue 23) pp:8180-8186
Publication Date(Web):May 19, 2010
DOI:10.1021/ja102777p
Graphite oxide sheet, now called graphene oxide (GO), is the product of chemical exfoliation of graphite and has been known for more than a century. GO has been largely viewed as hydrophilic, presumably due to its excellent colloidal stability in water. Here we report that GO is an amphiphile with hydrophilic edges and a more hydrophobic basal plane. GO can act like a surfactant, as measured by its ability to adsorb on interfaces and lower the surface or interfacial tension. Since the degree of ionization of the edge −COOH groups is affected by pH, GO’s amphiphilicity can be tuned by pH. In addition, size-dependent amphiphilicity of GO sheets is observed. Since each GO sheet is a single molecule as well as a colloidal particle, the molecule−colloid duality makes it behave like both a molecular and a colloidal surfactant. For example, GO is capable of creating highly stable Pickering emulsions of organic solvents like solid particles. It can also act as a molecular dispersing agent to process insoluble materials such as graphite and carbon nanotubes in water. The ease of its conversion to chemically modified graphene could enable new opportunities in solution processing of functional materials.
Co-reporter:Jiayan Luo ; Laura J. Cote ; Vincent C. Tung ; Alvin T. L. Tan ; Philip E. Goins ; Jinsong Wu
Journal of the American Chemical Society 2010 Volume 132(Issue 50) pp:17667-17669
Publication Date(Web):November 24, 2010
DOI:10.1021/ja1078943
Graphene oxide (GO) nanocolloids—sheets with lateral dimension smaller than 100 nm—were synthesized by chemical exfoliation of graphite nanofibers, in which the graphene planes are coin-stacked along the length of the nanofibers. Since the upper size limit is predetermined by the diameter of the nanofiber precursor, the size distribution of the GO nanosheets is much more uniform than that of common GO synthesized from graphite powders. The size can be further tuned by the oxidation time. Compared to the micrometer-sized, regular GO sheets, nano GO has very similar spectroscopic characteristics and chemical properties but very different solution properties, such as surface activity and colloidal stability. Due to higher charge density originating from their higher edge-to-area ratios, aqueous GO nanocolloids are significantly more stable. Dispersions of GO nanocolloids can sustain high-speed centrifugation and remain stable even after chemical reduction, which would result in aggregates for regular GO. Therefore, nano GO can act as a better dispersing agent for insoluble materials (e.g., carbon nanotubes) in water, creating a more stable colloidal dispersion.
Co-reporter:Franklin Kim;Jiayan Luo;Rodolfo Cruz-Silva;Laura J. Cote;Kwonnam Sohn
Advanced Functional Materials 2010 Volume 20( Issue 17) pp:2867-2873
Publication Date(Web):
DOI:10.1002/adfm.201000736

Abstract

Graphite oxide (GO) has received extensive interest as a precursor for the bulk production of graphene-based materials. Here, the highly energetic nature of GO, noted from the self-propagating thermal deoxygenating reaction observed in solid state, is explored. Although the resulting graphene product is quite stable against combustion even in a natural gas flame, its thermal stability is significantly reduced when contaminated with potassium salt by-products left from GO synthesis. In particular, the contaminated GO becomes highly flammable. A gentle touch with a hot soldering iron can trigger violent, catastrophic, total combustion of such GO films, which poses a serious fire hazard. This highlights the need for efficient sample purification methods. Typically, purification of GO is hindered by its tendency to gelate as the pH value increases during rinsing. A two-step, acid–acetone washing procedure is found to be effective for suppressing gelation and thus facilitating purification. Salt-induced flammability is alarming for the fire safety of large-scale manufacturing, processing, and storage of GO materials. However, the energy released from the deoxygenation of GO can also be harnessed to drive new reactions for creating graphene-based hybrid materials. Through such domino-like reactions, graphene sheets decorated with metal and metal oxide particles are synthesized using GO as the in situ power source. Enhanced electrochemical capacitance is observed for graphene sheets loaded with RuO2 nanoparticles.

Co-reporter:Franklin Kim;Jiayan Luo;Rodolfo Cruz-Silva;Laura J. Cote;Kwonnam Sohn
Advanced Functional Materials 2010 Volume 20( Issue 17) pp:
Publication Date(Web):
DOI:10.1002/adfm.201090077

Abstract

Graphite oxide (GO) has received extensive interest as a precursor for the bulk production of graphene-based materials. Here, the highly energetic nature of GO, noted from the self-propagating thermal deoxygenating reaction observed in solid state, is explored. Although the resulting graphene product is quite stable against combustion even in a natural gas flame, its thermal stability is significantly reduced when contaminated with potassium salt by-products left from GO synthesis. In particular, the contaminated GO becomes highly flammable. A gentle touch with a hot soldering iron can trigger violent, catastrophic, total combustion of such GO films, which poses a serious fire hazard. This highlights the need for efficient sample purification methods. Typically, purification of GO is hindered by its tendency to gelate as the pH value increases during rinsing. A two-step, acid–acetone washing procedure is found to be effective for suppressing gelation and thus facilitating purification. Salt-induced flammability is alarming for the fire safety of large-scale manufacturing, processing, and storage of GO materials. However, the energy released from the deoxygenation of GO can also be harnessed to drive new reactions for creating graphene-based hybrid materials. Through such domino-like reactions, graphene sheets decorated with metal and metal oxide particles are synthesized using GO as the in situ power source. Enhanced electrochemical capacitance is observed for graphene sheets loaded with RuO2 nanoparticles.

Co-reporter:Laura J. Cote, Jaemyung Kim, Zhen Zhang, Cheng Sun and Jiaxing Huang  
Soft Matter 2010 vol. 6(Issue 24) pp:6096-6101
Publication Date(Web):25 Sep 2010
DOI:10.1039/C0SM00667J
Graphene oxide (GO) sheets are a unique type of soft building block for creating functional graphene based materials and devices. Rapid progress has been made in the chemistry and applications of GO. However, there is a pressing need for rational assembly strategies of these two-dimensional (2D) sheets, which is crucial for determining the microstructures and thus final properties of bulk GO or graphene materials. For example, wrinkles and overlaps are the two fundamental morphologies between flexible, interacting sheets that are usually convoluted in solution-processed thin films. Based on the recent discovery of the surfactant-like property of GO sheets and their pH dependent amphiphilicity, now we are able to control the tiling of such 2D sheets to obtain thin films with either a wrinkled or overlapped type of microstructure, thus allowing us to deconvolute how these two basic microstructures affect the electrical and optical properties of the final thin films. The work here provides a well-defined example of the materials science paradigm, the microstructure-properties relationship, for this new soft material.
Co-reporter:Yong Sheng Zhao, Peng Zhan, Jaemyung Kim, Cheng Sun and Jiaxing Huang
ACS Nano 2010 Volume 4(Issue 3) pp:1630
Publication Date(Web):February 8, 2010
DOI:10.1021/nn901567z
Vertical nanowire arrays were prepared from an organic dye compound, 1,5-diaminoanthraquinone (DAAQ), on various types of substrates by a facile physical vapor transport method. It was found that the DAAQ grows much faster on the substrates with higher surface energies. Therefore, patterned growth of the nanowire arrays was achieved by modifying the substrate surfaces both geometrically and chemically to induce selective growth in areas of higher surface energies. The DAAQ nanowires can serve as nanosized active optical waveguides that allow the locally excited photoluminescence to propagate along the length of the wires. The low-loss waveguide propagation modes along the nanowire were observed experimentally. The nanowire arrays can be integrated directly with a portable fiber optics spectrometer for chemical vapor sensing.Keywords: chemical sensor; organic nanowire; patterning; vertical array; waveguide
Co-reporter:Laura J. Cote ; Rodolfo Cruz-Silva
Journal of the American Chemical Society 2009 Volume 131(Issue 31) pp:11027-11032
Publication Date(Web):July 14, 2009
DOI:10.1021/ja902348k
Graphite oxide (GO) is a promising precursor for the bulk production of graphene-based materials due to its relatively low cost of synthesis. The superior solvent processability of GO makes it particularly attractive for making composites by premixing with other materials. Typically, the reduction of GO has relied on either chemical agents or high temperature treatment. Here we report a room temperature, chemical-free flash reduction process where a photographic camera flash instantaneously triggers the deoxygenation reaction of GO by photothermal heating. Flash irradiation also rapidly creates a fused polymer composite from a random mixture of GO and polymer particles. Using a photomask, conducting patterns such as interdigitated electrode arrays can be readily made on flexible substrates.
Co-reporter:Kwonnam Sohn, Franklin Kim, Ken C. Pradel, Jinsong Wu, Yong Peng, Feimeng Zhou and Jiaxing Huang
ACS Nano 2009 Volume 3(Issue 8) pp:2191
Publication Date(Web):July 21, 2009
DOI:10.1021/nn900521u
In addition to chemical composition, the chemistry of nanocrystals involves an extra structural factor—morphology—since many of their properties are size- and shape-dependent. Although often described as artificial atoms or molecules, the morphological control of nanoparticles has not advanced to a level comparable to organic total synthesis, where complex molecular structures can be rationally designed and prepared through stepwise reactions. Here we report a morphological engineering approach for gold nanoparticles by constructing an evolutionary tree consisting of a few branches of independent growth pathways. Each branch yields a string of evolving, continuously tunable morphologies from one reaction, therefore collectively producing a library of nanoparticles with minimal changes of reaction parameters. In addition, the tree also provides ground rules for designing new morphologies through crossing over different pathways.Keywords: evolutionary tree; gold nanoparticle; nanorod; overgrowth
Co-reporter:Yu-Kyoung Oh, Jiaxing Huang
Advanced Drug Delivery Reviews (1 October 2016) Volume 105(Part B) pp:107-108
Publication Date(Web):1 October 2016
DOI:10.1016/j.addr.2016.09.008
Co-reporter:Kwonnam Sohn, Yoon Joo Na, Hankwon Chang, Ki-Min Roh, Hee Dong Jang and Jiaxing Huang
Chemical Communications 2012 - vol. 48(Issue 48) pp:NaN5970-5970
Publication Date(Web):2012/04/17
DOI:10.1039/C2CC32049E
Oil absorbing graphene capsules are synthesized by capillary molding of graphene oxide (GO) sheets against a polystyrene bead template in evaporating aerosol droplets, followed by simultaneous reduction of GO and decomposition of the polymer template during ultrasonic spray pyrolysis.
Co-reporter:Jiayan Luo, Vincent C. Tung, Andrew R. Koltonow, Hee Dong Jang and Jiaxing Huang
Journal of Materials Chemistry A 2012 - vol. 22(Issue 26) pp:NaN12996-12996
Publication Date(Web):2012/05/04
DOI:10.1039/C2JM30819C
An adhesive and conductive glue was created by synergistic assembly of graphene oxide (GO), single walled carbon nanotubes (SWCNTs) and conjugate polymer PEDOT:PSS in aqueous solution. The GO–SWCNTs–PEDOT:PSS glue can be used as a binder to fabricate metal oxide nanoparticle based ultracapacitors. Since the functional nanoparticles are immersed in this conductive gel, uniform electrical and mechanical interconnect can be achieved, leading to enhanced performance of ultracapacitors.
3,6,9,12-Tetraoxatricos-22-en-1-ol
3,6,9,12-Tetraoxatricosan-1-ol, 23-mercapto-
3',6'-Dihydroxy-3H-spiro[isobenzofuran-1,9'-xanthen]-3-one