Ruthenium/Graphene-like Layered Carbon Composite as an Efficient Hydrogen Evolution Reaction Electrocatalyst.

Efficient water splitting through electrocatalysis has been studied extensively in modern energy devices, while the development of catalysts with activity and stability comparable to those of Pt is still a great challenge. In this work, we successfully developed a facile route to synthesize graphene-like layered carbon (GLC) from a layered silicate template. The obtained GLC has layered structure similar to that of the template and can be used as support to load ultrasmall Ru nanoparticles on it in supercritical water. The specific structure and surface properties of GLC enable Ru nanoparticles to disperse highly uniformly on it even at a large loading amount (62 wt %). When the novel Ru/GLC was used as catalyst on a glass carbon electrode for hydrogen evolution reaction (HER) in a 0.5 M H2SO4 solution, it exhibits an extremely low onset potential of only 3 mV and a small Tafel slope of 46 mV/decade. The outstanding performance proved that Ru/GLC is highly active catalyst for HER, comparable with transition-metal dichalcogenides or selenides. As the price of ruthenium is much lower than platinum, our study shows that Ru/GLC might be a promising candidate as an HER catalyst in future energy applications.

[1]  Kun Xu,et al.  Free-Standing Two-Dimensional Ru Nanosheets with High Activity toward Water Splitting , 2016 .

[2]  K. Ayers,et al.  Ultralow charge-transfer resistance with ultralow Pt loading for hydrogen evolution and oxidation using Ru@Pt core-shell nanocatalysts , 2015, Scientific Reports.

[3]  Jong‐Min Lee,et al.  Platinum nanocuboids supported on reduced graphene oxide as efficient electrocatalyst for the hydrogen evolution reaction , 2015 .

[4]  X. Xia,et al.  Hot electron of Au nanorods activates the electrocatalysis of hydrogen evolution on MoS2 nanosheets. , 2015, Journal of the American Chemical Society.

[5]  Shouheng Sun,et al.  A New Core/Shell NiAu/Au Nanoparticle Catalyst with Pt-like Activity for Hydrogen Evolution Reaction. , 2015, Journal of the American Chemical Society.

[6]  X. Lou,et al.  Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production , 2015, Nature Communications.

[7]  Yong Wang,et al.  In situ cobalt-cobalt oxide/N-doped carbon hybrids as superior bifunctional electrocatalysts for hydrogen and oxygen evolution. , 2015, Journal of the American Chemical Society.

[8]  Yao Zheng,et al.  Advancing the electrochemistry of the hydrogen-evolution reaction through combining experiment and theory. , 2015, Angewandte Chemie.

[9]  N. Danilovic,et al.  Using surface segregation to design stable Ru-Ir oxides for the oxygen evolution reaction in acidic environments. , 2014, Angewandte Chemie.

[10]  Hui Zhu,et al.  Amorphous carbon supported MoS₂ nanosheets as effective catalysts for electrocatalytic hydrogen evolution. , 2014, Nanoscale.

[11]  Xile Hu,et al.  Nanostructured hydrotreating catalysts for electrochemical hydrogen evolution. , 2014, Chemical Society reviews.

[12]  Z. Tang,et al.  Noble Metal Nanoparticle@Metal Oxide Core/Yolk‐Shell Nanostructures as Catalysts: Recent Progress and Perspective , 2014 .

[13]  Abdullah M. Asiri,et al.  Carbon nanotubes decorated with CoP nanocrystals: a highly active non-noble-metal nanohybrid electrocatalyst for hydrogen evolution. , 2014, Angewandte Chemie.

[14]  H. Gasteiger,et al.  New insights into the electrochemical hydrogen oxidation and evolution reaction mechanism , 2014 .

[15]  Z. Yin,et al.  MoS2 nanoflower-decorated reduced graphene oxide paper for high-performance hydrogen evolution reaction. , 2014, Nanoscale.

[16]  Peter Strasser,et al.  Particle size effects in the catalytic electroreduction of CO₂ on Cu nanoparticles. , 2014, Journal of the American Chemical Society.

[17]  Yi Cui,et al.  CoSe2 nanoparticles grown on carbon fiber paper: an efficient and stable electrocatalyst for hydrogen evolution reaction. , 2014, Journal of the American Chemical Society.

[18]  James R. McKone,et al.  Nanostructured nickel phosphide as an electrocatalyst for the hydrogen evolution reaction. , 2013, Journal of the American Chemical Society.

[19]  R. Acres,et al.  Self-terminating protocol for an interfacial complexation reaction in vacuo by metal-organic chemical vapor deposition. , 2013, ACS nano.

[20]  James R. McKone,et al.  Ni–Mo Nanopowders for Efficient Electrochemical Hydrogen Evolution , 2013 .

[21]  Ya‐Wen Zhang,et al.  Ru nanocrystals with shape-dependent surface-enhanced Raman spectra and catalytic properties: controlled synthesis and DFT calculations. , 2012, Journal of the American Chemical Society.

[22]  M. Antonietti,et al.  Synthesis of monolayer-patched graphene from glucose. , 2012, Angewandte Chemie.

[23]  T. Jaramillo,et al.  Core-shell MoO3-MoS2 nanowires for hydrogen evolution: a functional design for electrocatalytic materials. , 2011, Nano letters.

[24]  Takahiko Moteki,et al.  Role of Acidic Pretreatment of Layered Silicate RUB-15 in Its Topotactic Conversion into Pure Silica Sodalite , 2011 .

[25]  Guosong Hong,et al.  MoS2 nanoparticles grown on graphene: an advanced catalyst for the hydrogen evolution reaction. , 2011, Journal of the American Chemical Society.

[26]  H. Dai,et al.  Solvothermal reduction of chemically exfoliated graphene sheets. , 2009, Journal of the American Chemical Society.

[27]  Takahiko Moteki,et al.  Silica sodalite without occluded organic matters by topotactic conversion of lamellar precursor. , 2008, Journal of the American Chemical Society.

[28]  Thomas F. Jaramillo,et al.  Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts , 2007, Science.

[29]  J. Nørskov,et al.  Computational high-throughput screening of electrocatalytic materials for hydrogen evolution , 2006, Nature materials.

[30]  Yong Wang,et al.  Fabrication of Ruthenium–Carbon Nanotube Nanocomposites in Supercritical Water , 2005 .

[31]  Thomas Bligaard,et al.  Trends in the exchange current for hydrogen evolution , 2005 .

[32]  H. Gies,et al.  A Layer Silicate: Synthesis and Structure of the Zeolite Precursor RUB‐15—[N(CH3)4]8[Si24O52(OH)4]·20 H2O , 1996 .

[33]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[34]  E. Sato,et al.  Electrocatalytic properties of transition metal oxides for oxygen evolution reaction , 1986 .

[35]  Micheál D. Scanlon,et al.  A nanoporous molybdenum carbide nanowire as an electrocatalyst for hydrogen evolution reaction , 2014 .