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Title: Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution

Abstract

One of the key components of carbon dioxide-free hydrogen production is a robust and efficient non-precious metal catalyst for the hydrogen evolution reaction. We report that a hierarchical nanoporous copper-titanium bimetallic electrocatalyst is able to produce hydrogen from water under a mild overpotential at more than twice the rate of state-of-the- art carbon-supported platinum catalyst. Although both copper and titanium are known to be poor hydrogen evolution catalysts, the combination of these two elements creates unique copper-copper-titanium hollow sites, which have a hydrogen-binding energy very similar to that of platinum, resulting in an exceptional hydrogen evolution activity. Moreover, the hierarchical porosity of the nanoporous-copper titanium catalyst also contributes to its high hydrogen evolution activity, because it provides a large-surface area for electrocatalytic hydrogen evolution, and improves the mass transport properties. Moreover, the catalyst is self-supported, eliminating the overpotential associated with the catalyst/support interface.

Authors:
 [1]; ORCiD logo [2];  [3];  [2];  [2];  [4];  [2];  [2];  [2];  [4];  [2];  [2];  [3]
+ Show Author Affiliations
  1. Univ. of Delaware, Newark, DE (United States); Columbia Univ., New York, NY (United States)
  2. Univ. of Delaware, Newark, DE (United States)
  3. Columbia Univ., New York, NY (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1256016
Grant/Contract Number:  
FG02-13ER16381; SC0009476
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lu, Qi, Hutchings, Gregory S., Yu, Weiting, Zhou, Yang, Forest, Robert V., Tao, Runzhe, Rosen, Jonathan, Yonemoto, Bryan T., Cao, Zeyuan, Zheng, Haimei, Xiao, John Q., Jiao, Feng, and Chen, Jingguang G. Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution. United States: N. p., 2015. Web. doi:10.1038/ncomms7567.
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Lu, Qi, Hutchings, Gregory S., Yu, Weiting, Zhou, Yang, Forest, Robert V., Tao, Runzhe, Rosen, Jonathan, Yonemoto, Bryan T., Cao, Zeyuan, Zheng, Haimei, Xiao, John Q., Jiao, Feng, & Chen, Jingguang G. Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution. United States. https://doi.org/10.1038/ncomms7567
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Lu, Qi, Hutchings, Gregory S., Yu, Weiting, Zhou, Yang, Forest, Robert V., Tao, Runzhe, Rosen, Jonathan, Yonemoto, Bryan T., Cao, Zeyuan, Zheng, Haimei, Xiao, John Q., Jiao, Feng, and Chen, Jingguang G. Mon . "Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution". United States. https://doi.org/10.1038/ncomms7567. https://www.osti.gov/servlets/purl/1256016.
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@article{osti_1256016,
title = {Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution},
author = {Lu, Qi and Hutchings, Gregory S. and Yu, Weiting and Zhou, Yang and Forest, Robert V. and Tao, Runzhe and Rosen, Jonathan and Yonemoto, Bryan T. and Cao, Zeyuan and Zheng, Haimei and Xiao, John Q. and Jiao, Feng and Chen, Jingguang G.},
abstractNote = {One of the key components of carbon dioxide-free hydrogen production is a robust and efficient non-precious metal catalyst for the hydrogen evolution reaction. We report that a hierarchical nanoporous copper-titanium bimetallic electrocatalyst is able to produce hydrogen from water under a mild overpotential at more than twice the rate of state-of-the- art carbon-supported platinum catalyst. Although both copper and titanium are known to be poor hydrogen evolution catalysts, the combination of these two elements creates unique copper-copper-titanium hollow sites, which have a hydrogen-binding energy very similar to that of platinum, resulting in an exceptional hydrogen evolution activity. Moreover, the hierarchical porosity of the nanoporous-copper titanium catalyst also contributes to its high hydrogen evolution activity, because it provides a large-surface area for electrocatalytic hydrogen evolution, and improves the mass transport properties. Moreover, the catalyst is self-supported, eliminating the overpotential associated with the catalyst/support interface.},
doi = {10.1038/ncomms7567},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Mon Mar 16 00:00:00 EDT 2015},
month = {Mon Mar 16 00:00:00 EDT 2015}
}
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https://doi.org/10.1038/ncomms7567
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journal, October 2010

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Atomic origins of the high catalytic activity of nanoporous gold
journal, August 2012

  • Fujita, Takeshi; Guan, Pengfei; McKenna, Keith
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Powering the planet: Chemical challenges in solar energy utilization
journal, October 2006

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journal, April 2010

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Sustainable Hydrogen Production
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Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts
journal, July 2007

  • Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J.
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journal, July 2012

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    Surface‐Electron Coupling for Efficient Hydrogen Evolution
    journal, October 2019

    Hierarchical β-Mo 2 C Nanotubes Organized by Ultrathin Nanosheets as a Highly Efficient Electrocatalyst for Hydrogen Production
    journal, November 2015

    • Ma, Fei-Xiang; Wu, Hao Bin; Xia, Bao Yu
    • Angewandte Chemie International Edition, Vol. 54, Issue 51
    • DOI: 10.1002/anie.201508715

    Silica-Polypyrrole Hybrids as High-Performance Metal-Free Electrocatalysts for the Hydrogen Evolution Reaction in Neutral Media
    journal, June 2017

    • Feng, Jin-Xian; Xu, Han; Ye, Sheng-Hua
    • Angewandte Chemie International Edition, Vol. 56, Issue 28
    • DOI: 10.1002/anie.201702934

    Donor–Acceptor Nanocarbon Ensembles to Boost Metal‐Free All‐pH Hydrogen Evolution Catalysis by Combined Surface and Dual Electronic Modulation
    journal, November 2019

    • Yang, Meijia; Zhang, You; Jian, Junhua
    • Angewandte Chemie International Edition, Vol. 58, Issue 45
    • DOI: 10.1002/anie.201907826

    Investigation of the Support Effect in Atomically Dispersed Pt on WO 3− x for Utilization of Pt in the Hydrogen Evolution Reaction
    journal, November 2019

    • Park, Jinkyu; Lee, Seonggyu; Kim, Hee‐Eun
    • Angewandte Chemie International Edition, Vol. 58, Issue 45
    • DOI: 10.1002/anie.201908122

    Perovskite materials in energy storage and conversion: Perovskite materials in energy storage and conversion
    journal, May 2016

    • Zhu, Liang; Ran, Ran; Tadé, Moses
    • Asia-Pacific Journal of Chemical Engineering, Vol. 11, Issue 3
    • DOI: 10.1002/apj.2000

    Folic Acid Derived Bimetallic-Doped Hollow Carbon Nanostructures for Efficient Electrocatalytic Oxygen Evolution
    journal, September 2018

    • Wu, Yuhang; Lu, Mengting; Li, Yuwen
    • Chemistry - An Asian Journal, Vol. 13, Issue 21
    • DOI: 10.1002/asia.201801121

    IrO 2 and Pt Doped Mesoporous SnO 2 Nanospheres as Efficient Electrocatalysts for the Facile OER and HER
    journal, October 2018

    • Bhanja, Piyali; Mohanty, Bishnupad; Patra, Astam K.
    • ChemCatChem, Vol. 11, Issue 1
    • DOI: 10.1002/cctc.201801312

    Low‐Dimensional Metal‐Organic Frameworks and their Diverse Functional Roles in Catalysis
    journal, May 2019

    Hollow Bimetallic Zinc Cobalt Phosphosulfides for Efficient Overall Water Splitting
    journal, December 2018

    • Liang, Zuozhong; Yang, Zhiyuan; Dang, Jingshuang
    • Chemistry – A European Journal
    • DOI: 10.1002/chem.201804492

    Dinitrosyl iron complexes: From molecular electrocatalysts to electrodeposited‐film electrodes for hydrogen evolution reaction
    journal, May 2019

    • Lu, Shan; Chiang, Jin‐Cheng; Chiou, Tzung‐Wen
    • Journal of the Chinese Chemical Society, Vol. 66, Issue 9
    • DOI: 10.1002/jccs.201900147

    Two Synthesis Methods for Fe(III)@MOF‐5‐derived Porous Carbon Composites for Enhanced Phenol Hydroxylation
    journal, December 2019

    Graphdiyne-Supported NiCo 2 S 4 Nanowires: A Highly Active and Stable 3D Bifunctional Electrode Material
    journal, June 2017

    Synthesis of Hierarchical 4H/fcc Ru Nanotubes for Highly Efficient Hydrogen Evolution in Alkaline Media
    journal, June 2018

    3D Interdigitated Microsupercapacitors with Record Areal Cell Capacitance
    journal, April 2019

    Dopamine-assisted synthesis of rGO@NiPd@NC sandwich structure for highly efficient hydrogen evolution reaction
    journal, December 2019

    • Wang, Jiaqi; Bao, Jiehua; Zhou, Yuming
    • Journal of Solid State Electrochemistry, Vol. 24, Issue 1
    • DOI: 10.1007/s10008-019-04459-3

    Atomic-scale Pt clusters decorated on porous α-Ni(OH)2 nanowires as highly efficient electrocatalyst for hydrogen evolution reaction
    journal, May 2017

    Defective MoS2 electrocatalyst for highly efficient hydrogen evolution through a simple ball-milling method
    journal, September 2017

    Three dimensional carbon substrate materials for electrolysis of water
    journal, June 2018

    Efficient hydrogen evolution by ternary molybdenum sulfoselenide particles on self-standing porous nickel diselenide foam
    journal, September 2016

    • Zhou, Haiqing; Yu, Fang; Huang, Yufeng
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms12765

    Machine learning hydrogen adsorption on nanoclusters through structural descriptors
    journal, July 2018

    • Jäger, Marc O. J.; Morooka, Eiaki V.; Federici Canova, Filippo
    • npj Computational Materials, Vol. 4, Issue 1
    • DOI: 10.1038/s41524-018-0096-5

    Earth-abundant catalysts for electrochemical and photoelectrochemical water splitting
    journal, January 2017

    • Roger, Isolda; Shipman, Michael A.; Symes, Mark D.
    • Nature Reviews Chemistry, Vol. 1, Issue 1
    • DOI: 10.1038/s41570-016-0003

    Highly efficient hydrogen evolution from seawater by a low-cost and stable CoMoP@C electrocatalyst superior to Pt/C
    journal, January 2017

    • Ma, Yuan-Yuan; Wu, Cai-Xia; Feng, Xiao-Jia
    • Energy & Environmental Science, Vol. 10, Issue 3
    • DOI: 10.1039/c6ee03768b

    Nanostructured catalysts for electrochemical water splitting: current state and prospects
    journal, January 2016

    • Li, Xiumin; Hao, Xiaogang; Abudula, Abuliti
    • Journal of Materials Chemistry A, Vol. 4, Issue 31
    • DOI: 10.1039/c6ta02334g

    Tin nanoparticles decorated copper oxide nanowires for selective electrochemical reduction of aqueous CO 2 to CO
    journal, January 2016

    • Zhao, Yong; Wang, Caiyun; Wallace, Gordon G.
    • Journal of Materials Chemistry A, Vol. 4, Issue 27
    • DOI: 10.1039/c6ta04155h

    An interfacial engineering approach towards two-dimensional porous carbon hybrids for high performance energy storage and conversion
    journal, January 2017

    • Lu, Chenbao; Liu, Shaohua; Zhang, Fan
    • Journal of Materials Chemistry A, Vol. 5, Issue 4
    • DOI: 10.1039/c6ta09278k

    Direct deposition of MoSe 2 nanocrystals onto conducting substrates: towards ultra-efficient electrocatalysts for hydrogen evolution
    journal, January 2017

    • Damien, Dijo; Anil, Athira; Chatterjee, Dipanwita
    • Journal of Materials Chemistry A, Vol. 5, Issue 26
    • DOI: 10.1039/c6ta09645j

    Conducting polymer nanofiber-supported Pt alloys: unprecedented materials for methanol oxidation with enhanced electrocatalytic performance and stability
    journal, January 2017

    • Ghosh, Srabanti; Bera, Susmita; Bysakh, Sandip
    • Sustainable Energy & Fuels, Vol. 1, Issue 5
    • DOI: 10.1039/c7se00126f

    Amination of 1-hexanol on bimetallic AuPd/TiO 2 catalysts
    journal, January 2018

    • Ball, Madelyn R.; Wesley, Thejas S.; Rivera-Dones, Keishla R.
    • Green Chemistry, Vol. 20, Issue 20
    • DOI: 10.1039/c8gc02321b

    Quasi-single-crystalline CoO hexagrams with abundant defects for highly efficient electrocatalytic water oxidation
    journal, January 2018

    • Liang, Zuozhong; Huang, Zhehao; Yuan, Haitao
    • Chemical Science, Vol. 9, Issue 34
    • DOI: 10.1039/c8sc02294a

    On the role of hydroxide species in sulphur- and nitrogen-doped cobalt-based carbon catalysts for the oxygen evolution reaction
    journal, January 2018

    • Shahraei, Ali; Kuebler, Markus; Martinaiou, Ioanna
    • Journal of Materials Chemistry A, Vol. 6, Issue 44
    • DOI: 10.1039/c8ta05769a

    3D nanoporous Ni/V 2 O 3 hybrid nanoplate assemblies for highly efficient electrochemical hydrogen evolution
    journal, January 2018

    • Ming, Mei; Ma, Yuling; Zhang, Yun
    • Journal of Materials Chemistry A, Vol. 6, Issue 43
    • DOI: 10.1039/c8ta07701k

    Transition metal modification and carbon vacancy promoted Cr 2 CO 2 (MXenes): a new opportunity for a highly active catalyst for the hydrogen evolution reaction
    journal, January 2018

    • Cheng, Yu-Wen; Dai, Jian-Hong; Zhang, Yu-Min
    • Journal of Materials Chemistry A, Vol. 6, Issue 42
    • DOI: 10.1039/c8ta07749e

    A substrate-free Mo 2 C-based electrocatalyst by facile glucose-blowing for efficient hydrogen production
    journal, January 2019

    • Li, Xiao; Hu, Xiao-Li; Wang, Xin-Long
    • New Journal of Chemistry, Vol. 43, Issue 48
    • DOI: 10.1039/c9nj04598h

    Rational construction of macroporous CoFeP triangular plate arrays from bimetal–organic frameworks as high-performance overall water-splitting catalysts
    journal, January 2019

    • Zhang, Ling; Wang, Xingyue; Li, Ang
    • Journal of Materials Chemistry A, Vol. 7, Issue 29
    • DOI: 10.1039/c9ta05282h

    Screening alloy electrocatalysts by combining magnetron sputtering and scanning electrochemical microscopy
    journal, May 2019

    Enhanced hydrogen evolution reaction on hybrids of cobalt phosphide and molybdenum phosphide
    journal, March 2017

    • Fang, Si-Ling; Chou, Tsu-Chin; Samireddi, Satyanarayana
    • Royal Society Open Science, Vol. 4, Issue 3
    • DOI: 10.1098/rsos.161016

    Enhanced hydrogen evolution reaction catalyzed by carbon‐rich Mo 4.8 Si 3 C 0.6 /C/SiC nanocomposites via a PDC approach
    journal, September 2019

    • Feng, Yao; Yu, Zhaoju; Riedel, Ralf
    • Journal of the American Ceramic Society, Vol. 103, Issue 2
    • DOI: 10.1111/jace.16824

    Copper (0) Doping Makes Cobalt-Nickel Hydroxide a High-Efficiency Catalyst for Hydrogen Evolution Reaction
    journal, January 2018

    • Bai, Jingjing; Sun, Qiangqiang; Zhou, Meng
    • Journal of The Electrochemical Society, Vol. 165, Issue 13
    • DOI: 10.1149/2.0881813jes

    3D Self-Supported Fe-Doped Ni 2 P Nanosheet Arrays as Bifunctional Catalysts for Overall Water Splitting
    journal, August 2017

    • Li, Yingjie; Zhang, Haichuan; Jiang, Ming
    • Advanced Functional Materials, Vol. 27, Issue 37
    • DOI: 10.1002/adfm.201702513

    A Perovskite Electrocatalyst for Efficient Hydrogen Evolution Reaction
    journal, May 2016

    Hydrogen Evolution and Oxidation: Mechanistic Studies and Material Advances
    journal, December 2018

    • Tian, Xiaoyu; Zhao, Pengcheng; Sheng, Wenchao
    • Advanced Materials, Vol. 31, Issue 31
    • DOI: 10.1002/adma.201808066

    Unconventional Nickel Nitride Enriched with Nitrogen Vacancies as a High-Efficiency Electrocatalyst for Hydrogen Evolution
    journal, June 2018

    Silica-Polypyrrole Hybrids as High-Performance Metal-Free Electrocatalysts for the Hydrogen Evolution Reaction in Neutral Media
    journal, June 2017

    Surface‐Electron Coupling for Efficient Hydrogen Evolution
    journal, December 2019

    • Fu, Weiwei; Wang, Yanwei; Hu, Jisong
    • Angewandte Chemie International Edition, Vol. 58, Issue 49
    • DOI: 10.1002/anie.201908938

    3D Hierarchical Porous Mo 2 C for Efficient Hydrogen Evolution
    journal, April 2016

    Synergistic Nanotubular Copper-Doped Nickel Catalysts for Hydrogen Evolution Reactions
    journal, February 2018

    Bottom-up synthesis of fully sp 2 hybridized three-dimensional microporous graphitic frameworks as metal-free catalysts
    journal, January 2017

    • Talapaneni, Siddulu Naidu; Kim, Jaehoon; Je, Sang Hyun
    • Journal of Materials Chemistry A, Vol. 5, Issue 24
    • DOI: 10.1039/c7ta02733h

    Ru nanodendrites composed of ultrathin fcc/hcp nanoblades for the hydrogen evolution reaction in alkaline solutions
    journal, January 2018

    • Gao, Kai; Wang, Yao; Wang, Zhiwei
    • Chemical Communications, Vol. 54, Issue 36
    • DOI: 10.1039/c8cc01343h

    Multiscale porous molybdenum phosphide of honeycomb structure for highly efficient hydrogen evolution
    journal, January 2018

    • Hou, Mengjie; Teng, Xue; Wang, Jianying
    • Nanoscale, Vol. 10, Issue 30
    • DOI: 10.1039/c8nr04246b

    Facile charge transfer in fibrous PdPt bimetallic nanocube counter electrodes
    journal, January 2019

    • Ramli, Muhamad Adam; Saad, Siti Khatijah Md; Mawarnis, Elvy Rahmi
    • New Journal of Chemistry, Vol. 43, Issue 28
    • DOI: 10.1039/c9nj01673b

    Decorating WSe 2 nanosheets with ultrafine Ru nanoparticles for boosting electrocatalytic hydrogen evolution in alkaline electrolytes
    journal, January 2019

    • Zhao, Yuanmeng; Mao, Guixiang; Huang, Chaozhang
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 6
    • DOI: 10.1039/c9qi00293f

    High loading accessible active sites via designable 3D-printed metal architecture towards promoting electrocatalytic performance
    journal, January 2019

    • Chang, Shuai; Huang, Xiaolei; Aaron Ong, Chun Yee
    • Journal of Materials Chemistry A, Vol. 7, Issue 31
    • DOI: 10.1039/c9ta05161a

    Catalyst design by scanning probe block copolymer lithography
    journal, March 2018

    • Huang, Liliang; Chen, Peng-Cheng; Liu, Mohan
    • Proceedings of the National Academy of Sciences, Vol. 115, Issue 15
    • DOI: 10.1073/pnas.1800884115

    One-pot synthesis of in situ carbon-decorated Cu 3 P particles with enhanced electrocatalytic hydrogen evolution performance
    journal, October 2017

    • Pi, Mingyu; Yang, Tao; Wang, Shuxia
    • Journal of Materials Research, Vol. 33, Issue 5
    • DOI: 10.1557/jmr.2017.401

    Development of a Dinitrosyl Iron Complex Molecular Catalyst into a Hydrogen Evolution Cathode
    journal, October 2015

    • Chiou, Tzung-Wen; Lu, Tsai-Te; Wu, Ying-Hao
    • Angewandte Chemie International Edition, Vol. 54, Issue 49
    • DOI: 10.1002/anie.201508351

    An amorphous dual action electrocatalyst based on oxygen doped cobalt sulfide for the hydrogen and oxygen evolution reactions
    journal, January 2017

    • Sultana, Ummul K.; He, Tianwei; Du, Aijun
    • RSC Advances, Vol. 7, Issue 87
    • DOI: 10.1039/c7ra10394h

    An organic ligand promoting the electrocatalytic activity of cobalt oxide for the hydrogen evolution reaction
    journal, January 2019

    • Chen, Chien-Hong; Chiou, Tzung-Wen; Chang, Han-Chun
    • Sustainable Energy & Fuels, Vol. 3, Issue 9
    • DOI: 10.1039/c9se00371a

    The fabrication of Co:ZnS/CoS 2 heterostructure nanowires with a superior hydrogen evolution performance
    journal, January 2019

    • Yan, Shancheng; Wang, Ka; Wu, Qingxia
    • Sustainable Energy & Fuels, Vol. 3, Issue 10
    • DOI: 10.1039/c9se00398c

    Folded nanosheet-like Co0.85Se array for overall water splitting
    journal, January 2018

    • Wu, Zhengcui; Li, Jingjing; Zou, Zexian
    • Journal of Solid State Electrochemistry, Vol. 22, Issue 6
    • DOI: 10.1007/s10008-018-3885-3

    Unconventional Nickel Nitride Enriched with Nitrogen Vacancies as a High-Efficiency Electrocatalyst for Hydrogen Evolution
    journal, June 2018

    Quasi-single-crystalline CoO hexagrams with abundant defects for highly efficient electrocatalytic water oxidation
    journal, January 2018

    • Liang, Zuozhong; Huang, Zhehao; Yuan, Haitao
    • Chemical Science, Vol. 9, Issue 34
    • DOI: 10.1039/c8sc02294a

    Enhanced hydrogen evolution reaction on hybrids of cobalt phosphide and molybdenum phosphide
    journal, March 2017

    • Fang, Si-Ling; Chou, Tsu-Chin; Samireddi, Satyanarayana
    • Royal Society Open Science, Vol. 4, Issue 3
    • DOI: 10.1098/rsos.161016

    Bulk layered heterojunction as an efficient electrocatalyst for hydrogen evolution
    journal, March 2017

    Electrospun Carbon Nanofibers with Embedded Co-Ceria Nanoparticles for Efficient Hydrogen Evolution and Overall Water Splitting
    journal, February 2020

    • Woo, Seongwon; Lee, Jooyoung; Lee, Dong Sub
    • Materials, Vol. 13, Issue 4
    • DOI: 10.3390/ma13040856
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