Highly Selective Two-Electron Oxygen Reduction Catalyzed by Mesoporous Nitrogen-Doped Carbon

Electrochemical reduction of oxygen molecules can produce H2O2, which is an important chemical for a green and sustainable society; therefore, the development of catalysts for this reaction is necessary. We propose mesoporous nitrogen-doped carbon prepared from (1-methyl-1H-pyrrole-2-yl)methanol in the presence of a mesoporous SiO2 template (KIT-6). The nitrogen content of the resulting carbon can be controlled in the range of 0–10 at. % and all prepared samples have well-ordered mesopores with diameters of 3.4–4.0 nm. Electrochemical studies indicate the present materials have high catalytic activities with high selectivity toward H2O2 over 90%. Such high selectivity toward H2O2 is probably due to good mass transport in the catalyst layer, which is enhanced by the mesoporous structure.

[1]  Itai Panas,et al.  Single atom hot-spots at Au-Pd nanoalloys for electrocatalytic H2O2 production. , 2011, Journal of the American Chemical Society.

[2]  T. Hayakawa,et al.  High performance Pt-free cathode catalysts for polymer electrolyte membrane fuel cells prepared from widely available chemicals , 2014 .

[3]  Bo-Qing Xu,et al.  Mesoporous carbon material co-doped with nitrogen and iron (Fe–N–C): high-performance cathode catalyst for oxygen reduction reaction in alkaline electrolyte , 2014 .

[4]  Takeshi Onizawa,et al.  Direct and continuous production of hydrogen peroxide with 93 % selectivity using a fuel-cell system. , 2003, Angewandte Chemie.

[5]  Alfred B. Anderson,et al.  O2 reduction on graphite and nitrogen-doped graphite: experiment and theory. , 2006, The journal of physical chemistry. B.

[6]  Kwang S. Kim,et al.  Interconnected Pt-nanodendrite/DNA/reduced-graphene-oxide hybrid showing remarkable oxygen reduction activity and stability. , 2013, ACS nano.

[7]  Xiaodong Zhuang,et al.  Nitrogen-doped carbon nanosheets with size-defined mesopores as highly efficient metal-free catalyst for the oxygen reduction reaction. , 2014, Angewandte Chemie.

[8]  Wataru Ueda,et al.  Electrocatalysis of heat-treated cobalt-porphyrin/carbon for hydrogen peroxide formation , 2013 .

[9]  S. Miyata,et al.  Oxygen reduction activity of pyrolyzed polypyrroles studied by 15N solid-state NMR and XPS with principal component analysis , 2012 .

[10]  Juan Herranz,et al.  Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells. , 2011, Nature communications.

[11]  Svitlana Pylypenko,et al.  Bifunctional Oxygen Reduction Reaction Mechanism on Non-Platinum Catalysts Derived from Pyrolyzed Porphyrins , 2010 .

[12]  K. Ariga,et al.  Preparation and Characterization of Well‐Ordered Hexagonal Mesoporous Carbon Nitride , 2005 .

[13]  D. Zhao,et al.  Facile synthesis of mesoporous carbon nitrides using the incipient wetness method and the application as hydrogen adsorbent , 2011 .

[14]  Chi-Chang Hu,et al.  Novel synthesis of N-doped porous carbons from collagen for electrocatalytic production of H2O2 , 2012 .

[15]  A. Salvi,et al.  XPS determination of oxygen‐containing functional groups on carbon‐fibre surfaces and the cleaning of these surfaces , 1990 .

[16]  Kiyoyuki Terakura,et al.  Carbon Alloy Catalysts: Active Sites for Oxygen Reduction Reaction , 2008 .

[17]  F. Du,et al.  Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction , 2009, Science.

[18]  Gang Wu,et al.  High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt , 2011, Science.

[19]  Robert Schlögl,et al.  Structural characterization of N-containing activated carbon fibers prepared from a low softening point petroleum pitch and a melamine resin , 2002 .

[20]  Yoshio Takasu,et al.  High oxygen-reduction activity of silk-derived activated carbon , 2009 .

[21]  Sang Hoon Joo,et al.  Synthesis of highly ordered carbon molecular sieves via template-mediated structural transformation , 1999 .

[22]  S. Takenaka,et al.  Study of Direct Synthesis of Hydrogen Peroxide Acid Solutions at a Heat-Treated MnCl–Porphyrin/Activated Carbon Cathode from H2 and O2 , 2012 .

[23]  Tsutomu Aoki,et al.  Highly durable Pt-free fuel cell catalysts prepared by multi-step pyrolysis of Fe phthalocyanine and phenolic resin , 2014 .

[24]  Umit S. Ozkan,et al.  The role of nanostructure in nitrogen-containing carbon catalysts for the oxygen reduction reaction , 2006 .

[25]  M. Jaroniec,et al.  Characterization of mesoporous carbons synthesized with SBA-16 silica template , 2005 .

[26]  H Jahnke,et al.  Organic dyestuffs as catalysts for fuel cells. , 1976, Topics in current chemistry.

[27]  S. Moriya,et al.  Preparation of carbon alloy catalysts for polymer electrolyte fuel cells from nitrogen-containing rigid-rod polymers , 2010 .

[28]  C. Liang,et al.  Polypyrrole-based nitrogen-doped carbon replicas of SBA-15 and SBA-16 containing magnetic nanoparticles , 2008 .

[29]  Kwang S. Kim,et al.  Stable platinum nanoclusters on genomic DNA–graphene oxide with a high oxygen reduction reaction activity , 2013, Nature Communications.

[30]  Ib Chorkendorff,et al.  Enabling direct H2O2 production through rational electrocatalyst design. , 2013, Nature materials.

[31]  Tae-Wan Kim,et al.  MCM-48-like large mesoporous silicas with tailored pore structure: facile synthesis domain in a ternary triblock copolymer-butanol-water system. , 2005, Journal of the American Chemical Society.

[32]  Markus Antonietti,et al.  Mesoporous nitrogen-doped carbon for the electrocatalytic synthesis of hydrogen peroxide. , 2012, Journal of the American Chemical Society.

[33]  A. B. Fuertes.  Template synthesis of mesoporous carbons with a controlled particle size , 2003 .