Improved high-current-density hydrogen evolution reaction kinetics on single-atom Co embedded in an order pore-structured nitrogen assembly carbon support

Yu, Jiaqi; Yan, Yu; Lin, Yuemin; Liu, Hengzhou; Li, Yuting; Xie, Shaohua; Sun, Simin; Liu, Fudong; Zhang, Zhiguo; Li, Wenzhen; Oh, Jin-Su; Zhou, Lin; Qi, Long; Wang, Bin; Huang, Wenyu

doi:10.1039/d4nh00299g

Title: Improved high-current-density hydrogen evolution reaction kinetics on single-atom Co embedded in an order pore-structured nitrogen assembly carbon support

Journal Article · Tue Sep 10 00:00:00 UTC 2024 · Nanoscale Horizons

DOI: https://doi.org/10.1039/d4nh00299g · OSTI ID:2447875

Yu, Jiaqi ^[1]; Yan, Yu ^[2]; Lin, Yuemin ^[3]; Liu, Hengzhou ^[1];

^[4]; Xie, Shaohua ^[5]; Sun, Simin ^[1]; Liu, Fudong ^[5];

^[6];

^[1];

^[4]; Zhou, Lin ^[4];

^[4];

^[2];

^[4]

Iowa State Univ., Ames, IA (United States)
Univ. of Oklahoma, Norman, OK (United States)
Iowa State Univ., Ames, IA (United States); Zhejiang Univ., Hangzhou (China)
Ames Lab., and Iowa State Univ., Ames, IA (United States)
Univ. of California, Riverside, CA (United States)
Zhejiang Univ., Hangzhou (China)

Single-atom catalysis is a subcategory of heterogeneous catalysis with well-defined active sites. Numerous endeavors have been devoted to developing single-atom catalysts for industrially applicable catalysis, including the hydrogen evolution reaction (HER). High-current-density electrolyzers have been pursued for single-atom catalysts to increase active-site density and enhance mass transfer. Here, we reasoned that a single-atom metal embedded in nitrogen assembly carbon (NAC) catalysts with high single-atom density, large surface area, and ordered mesoporosity, could fulfil an industrially applicable HER. Among several different single-atom catalysts, the HER overpotential with the best performing Co-NAC reached a current density of 200 mA cm^-2 at 310 mV, which is relevant to industrially applicable current density. Density functional theory (DFT) calculations suggested feasible hydrogen binding on single-atom Co resulted in the promising HER activity over Co-NAC. The best-performing Co-NAC showed robust performance under alkaline conditions at a current density of 50 mA cm^-2 for 20 h in an H-cell and at a current density of 150 mA cm^-2 for 100 h in a flow cell.

View Journal Article

Cite

Export

Save

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-07CH11358; SC0012704; SC0018284

OSTI ID:: 2447875

Report Number(s):: IS-J--11,447

Journal Information:: Nanoscale Horizons, Journal Name: Nanoscale Horizons Journal Issue: 12 Vol. 9; ISSN 2055-6756

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Single‐Atom Catalysts for Electrocatalytic Applications Zhang, Qiaoqiao; Guan, Jingqi Advanced Functional Materials, Vol. 30, Issue 31 https://doi.org/10.1002/adfm.202000768	journal	June 2020
Design of Aligned Porous Carbon Films with Single‐Atom Co–N–C Sites for High‐Current‐Density Hydrogen Generation Liu, Rui; Gong, Zhichao; Liu, Jianbin Advanced Materials, Vol. 33, Issue 41 https://doi.org/10.1002/adma.202103533	journal	August 2021
Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MN _x Active Moieties Enable Enhanced ORR Performance Zhu, Chengzhou; Shi, Qiurong; Xu, Bo Z. Advanced Energy Materials, Vol. 8, Issue 29 https://doi.org/10.1002/aenm.201801956	journal	August 2018
General Synthetic Strategy to Ordered Mesoporous Carbon Catalysts with Single‐Atom Metal Sites for Electrochemical CO₂ Reduction Luo, Zhicheng; Yin, Zhouyang; Yu, Jiaqi Small, Vol. 18, Issue 16 https://doi.org/10.1002/smll.202107799	journal	March 2022
Highly efficient and anti-poisoning single-atom cobalt catalyst for selective hydrogenation of nitroarenes Lin, Yuemin; Nie, Renfeng; Li, Yuting Nano Research, Vol. 15, Issue 12 https://doi.org/10.1007/s12274-022-4294-6	journal	April 2022
Studies of activated carbons used in double-layer capacitors Qu, Deyang; Shi, Hang Journal of Power Sources, Vol. 74, Issue 1, p. 99-107 https://doi.org/10.1016/S0378-7753(98)00038-X	journal	July 1998
Soft X-ray absorption spectroscopy in heterogeneous catalysis Bazin, D.; Guczi, L. Applied Catalysis A: General, Vol. 213, Issue 2 https://doi.org/10.1016/S0926-860X(00)00895-4	journal	May 2001
Fischer–Tropsch synthesis: Temperature programmed EXAFS/XANES investigation of the influence of support type, cobalt loading, and noble metal promoter addition to the reduction behavior of cobalt oxide particles Jacobs, Gary; Ji, Yaying; Davis, Burtron H. Applied Catalysis A: General, Vol. 333, Issue 2 https://doi.org/10.1016/j.apcata.2007.07.027	journal	December 2007
Descriptors for Hydrogen Evolution on Single Atom Catalysts in Nitrogen-Doped Graphene Fung, Victor; Hu, Guoxiang; Wu, Zili The Journal of Physical Chemistry C, Vol. 124, Issue 36 https://doi.org/10.1021/acs.jpcc.0c04432	journal	August 2020
Highly Efficient Multifunctional Co–N–C Electrocatalysts with Synergistic Effects of Co–N Moieties and Co Metallic Nanoparticles Encapsulated in a N-Doped Carbon Matrix for Water-Splitting and Oxygen Redox Reactions Lyu, Dandan; Du, Yonghua; Huang, Shangli ACS Applied Materials & Interfaces, Vol. 11, Issue 43 https://doi.org/10.1021/acsami.9b11870	journal	September 2019
Engineering Low-Coordination Single-Atom Cobalt on Graphitic Carbon Nitride Catalyst for Hydrogen Evolution Liu, Xinghui; Deng, Yuchen; Zheng, Lirong ACS Catalysis, Vol. 12, Issue 9 https://doi.org/10.1021/acscatal.2c01253	journal	April 2022
Pt/Pd Single-Atom Alloys as Highly Active Electrochemical Catalysts and the Origin of Enhanced Activity Zhang, Lei; Liu, Hanshuo; Liu, Sihang ACS Catalysis, Vol. 9, Issue 10 https://doi.org/10.1021/acscatal.9b01677	journal	September 2019
Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction McCrory, Charles C. L.; Jung, Suho; Peters, Jonas C. Journal of the American Chemical Society, Vol. 135, Issue 45 https://doi.org/10.1021/ja407115p	journal	October 2013
Single Carbon Vacancy Traps Atomic Platinum for Hydrogen Evolution Catalysis Yang, Qin; Liu, Hanxuan; Yuan, Pei Journal of the American Chemical Society, Vol. 144, Issue 5 https://doi.org/10.1021/jacs.1c10814	journal	January 2022
Hybrid Catalyst Coupling Single-Atom Ni and Nanoscale Cu for Efficient CO₂ Electroreduction to Ethylene Yin, Zhouyang; Yu, Jiaqi; Xie, Zhenhua Journal of the American Chemical Society, Vol. 144, Issue 45 https://doi.org/10.1021/jacs.2c09773	journal	November 2022
C and N Hybrid Coordination Derived Co–C–N Complex as a Highly Efficient Electrocatalyst for Hydrogen Evolution Reaction Wang, Zhong-Li; Hao, Xian-Feng; Jiang, Zheng Journal of the American Chemical Society, Vol. 137, Issue 48 https://doi.org/10.1021/jacs.5b09021	journal	November 2015
Surface-Engineered PtNi-O Nanostructure with Record-High Performance for Electrocatalytic Hydrogen Evolution Reaction Zhao, Zipeng; Liu, Haotian; Gao, Wenpei Journal of the American Chemical Society, Vol. 140, Issue 29 https://doi.org/10.1021/jacs.8b04770	journal	June 2018
Structural and Electronic Optimization of MoS ₂ Edges for Hydrogen Evolution Wang, Hao; Xiao, Xu; Liu, Shuyuan Journal of the American Chemical Society, Vol. 141, Issue 46 https://doi.org/10.1021/jacs.9b09932	journal	November 2019
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode Nørskov, J. K.; Rossmeisl, J.; Logadottir, A. The Journal of Physical Chemistry B, Vol. 108, Issue 46 https://doi.org/10.1021/jp047349j	journal	November 2004
Anchoring zero valence single atoms of nickel and iron on graphdiyne for hydrogen evolution Xue, Yurui; Huang, Bolong; Yi, Yuanping Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03896-4	journal	April 2018
Pt-O bond as an active site superior to Pt0 in hydrogen evolution reaction Yu, Fei-Yang; Lang, Zhong-Ling; Yin, Li-Ying Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-019-14274-z	journal	January 2020
Mastering the surface strain of platinum catalysts for efficient electrocatalysis He, Tianou; Wang, Weicong; Shi, Fenglei Nature, Vol. 598, Issue 7879 https://doi.org/10.1038/s41586-021-03870-z	journal	October 2021
Phase-dependent growth of Pt on MoS2 for highly efficient H2 evolution Shi, Zhenyu; Zhang, Xiao; Lin, Xiaoqian Nature, Vol. 621, Issue 7978 https://doi.org/10.1038/s41586-023-06339-3	journal	September 2023
Fe–N–C electrocatalyst with dense active sites and efficient mass transport for high-performance proton exchange membrane fuel cells Wan, Xin; Liu, Xiaofang; Li, Yongcheng Nature Catalysis, Vol. 2, Issue 3 https://doi.org/10.1038/s41929-019-0237-3	journal	March 2019
Insight on Tafel slopes from a microkinetic analysis of aqueous electrocatalysis for energy conversion Shinagawa, Tatsuya; Garcia-Esparza, Angel T.; Takanabe, Kazuhiro Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep13801	journal	September 2015
A nanoporous molybdenum carbide nanowire as an electrocatalyst for hydrogen evolution reaction Liao, Lei; Wang, Sinong; Xiao, Jingjing Energy Environ. Sci., Vol. 7, Issue 1 https://doi.org/10.1039/C3EE42441C	journal	January 2014
Recent advances in heterogeneous electrocatalysts for the hydrogen evolution reaction Zeng, Min; Li, Yanguang Journal of Materials Chemistry A, Vol. 3, Issue 29 https://doi.org/10.1039/C5TA02974K	journal	January 2015
A cobalt–phosphorus nanoparticle decorated N-doped carbon nanosheet array for efficient and durable hydrogen evolution at alkaline pH Li, Xinyi; Zhang, Rong; Luo, Yongsong Sustainable Energy & Fuels, Vol. 4, Issue 8 https://doi.org/10.1039/D0SE00240B	journal	January 2020
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
Single-atomic cobalt sites embedded in hierarchically ordered porous nitrogen-doped carbon as a superior bifunctional electrocatalyst Sun, Tingting; Zhao, Shu; Chen, Wenxing Proceedings of the National Academy of Sciences, Vol. 115, Issue 50 https://doi.org/10.1073/pnas.1813605115	journal	November 2018
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Local Ordering Around Tetrahedral Co ²⁺ in Silicate Glasses Hunault, Myrtille; Calas, Georges; Galoisy, Laurence Journal of the American Ceramic Society, Vol. 97, Issue 1 https://doi.org/10.1111/jace.12709	journal	December 2013
Triblock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores Zhao, Dongyuan; Feng, Jianglin; Huo, Qisheng Science, Vol. 279, Issue 5350, p. 548-552 https://doi.org/10.1126/science.279.5350.548	journal	January 1998
Trends in the Exchange Current for Hydrogen Evolution Nørskov, J. K.; Bligaard, T.; Logadottir, A. Journal of The Electrochemical Society, Vol. 152, Issue 3 https://doi.org/10.1149/1.1856988	journal	January 2005
X-ray absorption near edge structures in cobalt oxides Jiang, T.; Ellis, D. E. Journal of Materials Research, Vol. 11, Issue 9 https://doi.org/10.1557/JMR.1996.0285	journal	September 1996

Similar Records

Highly Efficient Hydrogen Evolution from a Mesoporous Hybrid of Nickel Phosphide Nanoparticles Anchored on Cobalt Phosphosulfide/Phosphide Nanosheet Arrays

Journal Article · Sun Jan 13 00:00:00 UTC 2019 · Small · OSTI ID:1490762

Sun, Jingying; Ren, Muqing; Yu, Luo; +7 more

Co-Mo-P Based Electrocatalyst for Superior Reactivity in the Alkaline Hydrogen Evolution Reaction

Journal Article · Thu Oct 04 04:00:00 UTC 2018 · ChemCatChem · OSTI ID:1566405

Thenuwara, Akila C.; Dheer, Lakshay; Attanayake, Nuwan H.; +3 more

Amorphizing noble metal chalcogenide catalysts at the single-layer limit towards hydrogen production

Journal Article · Thu Mar 10 00:00:00 UTC 2022 · Nature Catalysis · OSTI ID:1887851

He, Yongmin; Liu, Liren; Zhu, Chao; +24 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Improved high-current-density hydrogen evolution reaction kinetics on single-atom Co embedded in an order pore-structured nitrogen assembly carbon support

Citation Formats

References (39)

Similar Records

Related Subjects