Abstract
Pt heterostructures can have distinctly different physical and chemical properties to their single-phase components. Herein, a smart approach was developed for the large-scale production of graphitic C3N4-Pt (gC3N4-Pt) heterostructures on three-dimensional (3D) graphene sheet networks for highly efficient methanol oxidation. Because the gC3N4-Pt heterostructures on the conductive 3D graphene network support provide the methanol molecules good accessibility to the active sites, the obtained catalyst exhibits excellent electrocatalytic performance, including high catalytic activity, unusual CO tolerance, and good stability, and is superior to commercial Pt/C and Pt/graphene catalysts for methanol oxidation.
中文摘要
Pt基异质结构具有与单一相材料不同的物理和化学性质. 本研究巧妙地设计了一种非金属gC3N4和Pt的异质结构, 并将其负载在三维石墨烯网状结构上作为甲醇氧化的催化剂. 由于Pt和gC3N4之间的协同作用, 结合三维多孔石墨烯作为导电载体, 为活性位点接触燃料分子提供了最大限度的可能, 使得到的催化剂表现出异常优越的性能, 包括高的催化活性, 不同寻常的抗CO中毒能力, 以及良好的稳定性. 这些性能优于商业化的碳负载Pt催化剂以及三维石墨烯 负载Pt催化剂.
Article PDF
Similar content being viewed by others
References
Zhang S, Shao YY, Yin GP, Lin YH. Electrostatic self-assembly of a Pt-around-Au nanocomposite with high activity towards formic acid oxidation. Angew Chem Int Ed, 2010, 49: 1–5
Wang L, Nemoto Y, Yamauchi Y. Direct synthesis of spatially-controlled Pt-on-Pd bimetallic nanodendrites with superior electrocatalytic activity. J Am Chem Soc, 2011, 133: 9674–9677
Sasaki K, Naohara H, Cai Y, et al. Core-protected platinum monolayer shell high-stability electrocatalysts for fuel-cell cathodes. Angew Chem, 2010, 122: 8784–8789
Yang JH, Yang J, Ying JY. Morphology and lateral strain control of Pt nanoparticles via core-shell construction using alloy AgPd core toward oxygen reduction reaction. ACS Nano, 2012, 6: 9373–9382
An K, Alayoglu S, Musselwhite N, et al. Enhanced CO oxidation rates at the interface of mesoporous oxides and Pt nanoparticles, J Am Chem Soc, 2013, 135: 16689–16696
Yang J, Ying JY. Nanocomposites of Ag2S and noble metals. Angew Chem Int Ed, 2011, 50: 4637–4643
Chung LL, Yang J, Wei Y, Ying JY. Semiconductor-gold nanocomposite catalysts for the efficient three-component coupling of aldehyde, amine and alkyne in water. Adv Synth Catal, 2009, 351: 2887–2896
Lin ZZ, Wang XC. Nanostructure engineering and doping of conjugated carbon nitride semiconductors for hydrogen photosynthesis. Angew Chem Int Ed, 2013, 52: 1735–1738
Wang X, Maeda K, Thomas A, et al. A metal-free polymeric photo-catalyst for hydrogen production from water under visible light. Nat Mater, 2009, 8: 76–80
Xu K, Li XL, Chen PZ, et al. Hydrogen dangling bonds induce ferromagnetism in two-dimensional metal-free graphitic-C3N4 nanosheets. doi: 10.1039/c4sc02576h
Hu CG, Song L, Zhang ZP, et al. Tailored graphene systems for unconventional applications in energy conversion and storage devices. doi: 10.1039/c4ee02594f
Shao Y, Zhang S, Wang C, et al. Highly durable graphene nanoplatelets supported Pt nanocatalysts for oxygen reduction, J Power Sources, 2010, 195: 4600–4605
Hu CG, Zhao Y, Cheng HH, et al. Ternary Pd2/PtFe networks supported by 3D graphene for efficient and durable electrooxidation of formic acid. Chem Commun, 2012, 48: 11865–11867
Yu D, Dai L. Self-assembled graphene/carbon nano-tube hybrid films for supercapacitors. J Phys Chem Lett, 2010, 1: 467–470
Xu YX, Sheng KX, Li C, Shi GQ. Self-assembled graphene hydrogel via a one-step hydrothermal process. ACS Nano, 2010, 4: 4324–4330
Zhang SW, Li JX, Zeng MY, et al. Polymer nanodots of graphitic carbon nitride as effective fluorescent probes for the detection of Fe3+ and Cu2+ ions. Nanoscale, 2014, 6: 4157–4162
Hu CG, Cheng HH, Zhao Y, et al. Newly-designed complex ternary Pt/PdCu nanoboxes anchored on three-dimensional graphene framework for highly efficient ethanol oxidation. Adv Mater, 2012, 24: 5493–5498
Li YH, Hung TH, Chen CW. A first-principles study of nitrogen-and boron-assisted platinum adsorption on carbon nanotubes. Carbon, 2009, 47: 850–855
Zhou Y, Neyerlin K, Olson TS, et al. Enhancement of Pt and Pt-alloy fuel cell catalyst activity and durability via nitrogen-modified carbon supports. Energy Environ Sci, 2010, 3: 1437–1446
Hu CG, Cao YX, Yang L, et al. Preparation of highly dispersed Pt-SnOx nanoparticles supported on multi-walled carbon nanotubes for methanol oxidation. Appl Surf Sci, 2011, 257: 7968–7974
Zhao D, Xu BQ. Enhancement of Pt utilization in electrocatalysts by using gold nanoparticles. Angew Chem Int Ed, 2006, 45: 4955–4959
Hu CG, Zhai XQ, Liu LI, et al. Spontaneous reduction and assembly of graphene oxide into three-dimensional graphene network on arbitrary conductive substrates. Sci Rep, 2013, 3: 2065–2074
Hu CG, Xiao Y, Zhao Y, et al. Highly nitrogen-doped carbon capsules: scalable preparation and high-performance applications in fuel cells and lithium ion batteries. Nanoscale, 2013, 5: 2726–2733
Vinu A. Two-dimensional hexagonally-ordered mesoporous carbon nitrides with tunable pore diameter, surface area and nitrogen content. Adv Funct Mater, 2008, 18: 816–827
Cui Y, Zhang J, Zhang G, et al. Synthesis of bulk and nanoporous carbon nitride polymers from ammonium thiocyanate for photo catalytic hydrogen evolution. J Mater Chem, 2011, 21: 13032–13039
Li YH, Hung TH, Chen CW. A first-principles study of nitrogen- and boron-assisted platinum adsorption on carbon nanotubes. Carbon, 2009, 47: 850–855
Pan C, Qiu L, Peng Y, et al. Facile synthesis of nitrogen-doped carbon-Pt nanoparticle hybrids via carbonization of poly ([Bvim] [Br]-co-acrylonitrile) for electrocatalytic oxidation of methanol. J Mater Chem, 2012, 22: 13578–13584
Hu CG, Zheng GP, Zhao F, et al. A powerful approach to functional graphene hybrids for high performance energy-related applications. Energy Environ Sci, 2014, 7: 3699–3708
Hu CG, Guo YM, Cao YX, et al. A facile method for preparation of high performance Pt catalyst supported on multi-wall carbon nanotubes for methanol electrooxidation. Mater Sci Eng B, 2011, 176: 1467–1473
Kuang Y, Cai Z, Zhang Y, et al. Ultrathin dendritic Pt3Cu triangular pyramid caps with enhanced electrocatalytic activity. ACS Appl Mater Interfaces, 2014, 6: 17748–17752
Li YJ, Gao W, Ci LJ, et al. Catalytic performance of Pt nanoparticles on reduced graphene oxide for methanol electro-oxidation. Carbon, 2010, 48: 1124–1130
Cai Z, Kuang Y, Qi XH, et al. Ultrathin branched PtFe and PtRuFe nanodendrites with enhanced electrocatalytic activity. J Mater Chem A, doi: 10.1039/c4ta04698f
Yang G, Li Y, Rana RK, Zhu JJ. Pt-Au/nitrogen-doped graphene nanocomposites for enhanced electrochemical activities. J Mater Chem A, 2013, 1: 1754–1762
Ferreira PG, la O’ PG, Shao-Horn Y, et al. Instability of Pt/C electrocatalysts in proton exchange membrane fuel cells-amechanistic investigation. J Electrochem Soc, 2005, 152: A2256–A2271
Wang C, Vliet D, More K, et al. Multimetallic Au/FePt3 nanoparticles as highly durable electrocatalyst. Nano Lett, 2011, 11: 919–926
Kim P, Kim HS, Joo JB, et al. Preparation and application of nanoporous carbon templated by silica particle for use as a catalyst support for direct methanol fuel cell. J Power Sources, 2005, 145: 139–146
Author information
Authors and Affiliations
Corresponding author
Additional information
Chuangang Hu is a PhD student from the research group of functional nanostructures supervised by Professor Liangti Qu at Beijing Institute of Technology. His research focuses on the functionalization of graphenes for energy conversion and storage applications.
Liangti Qu received a PhD in chemistry from Tsinghua University (Beijing, China) in 2004. He became a professor of chemistry at Beijing Institute of Technology in 2009 after working at the University of Dayton (Ohio, USA) for 5 years. As the Xu-Teli Distinguished Professor, he now leads the nanocarbon research group. This group is interested in materials chemistry, mainly focusing on the synthesis, functionalization, and application of nanomaterials with carbon-carbon conjugated structures including graphenes, carbon nanotubes, and conducting polymers.
Electronic supplementary material
Rights and permissions
About this article
Cite this article
Hu, C., Han, Q., Zhao, F. et al. Graphitic C3N4-Pt nanohybrids supported on a graphene network for highly efficient methanol oxidation. Sci. China Mater. 58, 21–27 (2015). https://doi.org/10.1007/s40843-014-0012-3
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s40843-014-0012-3