Gel‐Derived Amorphous Bismuth–Nickel Alloy Promotes Electrocatalytic Nitrogen Fixation via Optimizing Nitrogen Adsorption and Activation

Fang, Zhiwei; Wu, Ping; Qian, Yumin; Yu, Guihua

doi:10.1002/ange.202014302

Gel‐Derived Amorphous Bismuth–Nickel Alloy Promotes Electrocatalytic Nitrogen Fixation via Optimizing Nitrogen Adsorption and Activation

Journal Article · Wed Dec 23 00:00:00 EST 2020 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202014302· OSTI ID:1782389

Fang, Zhiwei ^[1]; Wu, Ping ^[2]; Qian, Yumin ^[1]; ^[1]

Materials Science and Engineering Program Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA
Materials Science and Engineering Program Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA, Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Center of Biomedical Functional Materials School of Chemistry and Materials Science Nanjing Normal University Nanjing 210023 China

Abstract

To achieve the electrochemical nitrogen reduction reaction (NRR) for efficient and sustainable NH ₃ production, catalysts should exhibit high selectivity and activity with optimal adsorption energy. Herein we developed a three‐dimensional (3D) amorphous BiNi alloy toward a significantly enhanced NRR compared with its crystalline and metal counterparts. Ni alloying enables the chemisorption of nitrogen and the lower free‐energy change for the *NNH formation, and the 3D alloy electrocatalyst exhibits high catalytic activity for NH ₃ production with a yield rate of 17.5 μg h ⁻¹ mg _cat ⁻¹ and Faradaic efficiency of 13.8 %. The enhanced electron transfer and increased electrochemical surface area were revealed in the interconnected porous scaffold, affording it sufficiently efficient and stable activity for potential practical applications. This work offers new insights into optimizing the adsorption energy of reactants and intermediates combined with tuning the crystallinity of NRR electrocatalysts.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0019019

OSTI ID:: 1782389

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 8 Vol. 133; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (49)

Electrochemical Reduction of N ₂ under Ambient Conditions for Artificial N ₂ Fixation and Renewable Energy Storage Using N ₂ /NH ₃ Cycle Bao, Di; Zhang, Qi; Meng, Fan-Lu Advanced Materials, Vol. 29, Issue 3 https://doi.org/10.1002/adma.201604799	journal	November 2016
Amorphizing of Au Nanoparticles by CeO _x -RGO Hybrid Support towards Highly Efficient Electrocatalyst for N ₂ Reduction under Ambient Conditions Li, Si-Jia; Bao, Di; Shi, Miao-Miao Advanced Materials, Vol. 29, Issue 33 https://doi.org/10.1002/adma.201700001	journal	July 2017
Achieving a Record-High Yield Rate of 120.9 μgNH3 mgcat.−1 h−1 for N ₂ Electrochemical Reduction over Ru Single-Atom Catalysts Geng, Zhigang; Liu, Yan; Kong, Xiangdong Advanced Materials, Vol. 30, Issue 40 https://doi.org/10.1002/adma.201803498	journal	August 2018
Anchoring PdCu Amorphous Nanocluster on Graphene for Electrochemical Reduction of N ₂ to NH ₃ under Ambient Conditions in Aqueous Solution Shi, Miao-Miao; Bao, Di; Li, Si-Jia Advanced Energy Materials, Vol. 8, Issue 21 https://doi.org/10.1002/aenm.201800124	journal	April 2018
In Situ Fragmented Bismuth Nanoparticles for Electrocatalytic Nitrogen Reduction Yao, Dazhi; Tang, Cheng; Li, Laiquan Advanced Energy Materials, Vol. 10, Issue 33 https://doi.org/10.1002/aenm.202001289	journal	July 2020
An Amorphous Noble-Metal-Free Electrocatalyst that Enables Nitrogen Fixation under Ambient Conditions Lv, Chade; Yan, Chunshuang; Chen, Gang Angewandte Chemie, Vol. 130, Issue 21 https://doi.org/10.1002/ange.201801538	journal	March 2018
Defect Engineering Metal-Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions Lv, Chade; Qian, Yumin; Yan, Chunshuang Angewandte Chemie, Vol. 130, Issue 32 https://doi.org/10.1002/ange.201806386	journal	July 2018
Generating Defect‐Rich Bismuth for Enhancing the Rate of Nitrogen Electroreduction to Ammonia Wang, Yue; Shi, Miao‐miao; Bao, Di Angewandte Chemie, Vol. 131, Issue 28 https://doi.org/10.1002/ange.201903969	journal	May 2019
An Amorphous Noble-Metal-Free Electrocatalyst that Enables Nitrogen Fixation under Ambient Conditions Lv, Chade; Yan, Chunshuang; Chen, Gang Angewandte Chemie International Edition, Vol. 57, Issue 21 https://doi.org/10.1002/anie.201801538	journal	March 2018
Defect Engineering Metal-Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions Lv, Chade; Qian, Yumin; Yan, Chunshuang Angewandte Chemie International Edition, Vol. 57, Issue 32 https://doi.org/10.1002/anie.201806386	journal	July 2018
Generating Defect‐Rich Bismuth for Enhancing the Rate of Nitrogen Electroreduction to Ammonia Wang, Yue; Shi, Miao‐miao; Bao, Di Angewandte Chemie International Edition, Vol. 58, Issue 28 https://doi.org/10.1002/anie.201903969	journal	July 2019
Promotion Effect of Bismuth on Nickel Electrodeposition and Its Electrocatalysis to Glucose Oxidation Wu, Jiuyang; Miao, Yuqing; Liang, Xiaocai Electroanalysis, Vol. 26, Issue 4 https://doi.org/10.1002/elan.201300615	journal	March 2014
Defect Engineering Strategies for Nitrogen Reduction Reactions under Ambient Conditions Yan, Dafeng; Li, Hao; Chen, Chen Small Methods, Vol. 3, Issue 6 https://doi.org/10.1002/smtd.201800331	journal	October 2018
Nitrogen Reduction Reaction Zheng, Gengfeng; Yan, Jun‐Min; Yu, Guihua Small Methods, Vol. 3, Issue 6 https://doi.org/10.1002/smtd.201900070	journal	October 2018
Mo2C@3D ultrathin macroporous carbon realizing efficient and stable nitrogen fixation Fang, Zhiwei; Fernandez, Desiree; Wang, Nana Science China Chemistry, Vol. 63, Issue 11 https://doi.org/10.1007/s11426-020-9740-8	journal	April 2020
Bi-Ni (Bismuth-Nickel) Okamoto, H. Journal of Phase Equilibria and Diffusion, Vol. 33, Issue 6 https://doi.org/10.1007/s11669-012-0091-3	journal	July 2012
Amorphous engineered cerium oxides photocatalyst for efficient nitrogen fixation Zhang, Congmin; Xu, Yanling; Lv, Chade Applied Catalysis B: Environmental, Vol. 264 https://doi.org/10.1016/j.apcatb.2019.118416	journal	May 2020
Accelerated Dinitrogen Electroreduction to Ammonia via Interfacial Polarization Triggered by Single-Atom Protrusions Li, Jie; Chen, Shang; Quan, Fengjiao Chem, Vol. 6, Issue 4 https://doi.org/10.1016/j.chempr.2020.01.013	journal	April 2020
Boosting Electrocatalytic Ammonia Production through Mimicking “π Back-Donation” Lv, Chade; Zhong, Lixiang; Yao, Yao Chem, Vol. 6, Issue 10 https://doi.org/10.1016/j.chempr.2020.07.006	journal	October 2020
Electrocatalytic Nitrogen Reduction at Low Temperature Deng, Jiao; Iñiguez, Jesus A.; Liu, Chong Joule, Vol. 2, Issue 5 https://doi.org/10.1016/j.joule.2018.04.014	journal	May 2018
Solar Water Splitting and Nitrogen Fixation with Layered Bismuth Oxyhalides Li, Jie; Li, Hao; Zhan, Guangming Accounts of Chemical Research, Vol. 50, Issue 1 https://doi.org/10.1021/acs.accounts.6b00523	journal	December 2016
Hydrogels and Hydrogel-Derived Materials for Energy and Water Sustainability Guo, Youhong; Bae, Jiwoong; Fang, Zhiwei Chemical Reviews, Vol. 120, Issue 15 https://doi.org/10.1021/acs.chemrev.0c00345	journal	July 2020
Bimetallic Nanocrystals: Syntheses, Properties, and Applications Gilroy, Kyle D.; Ruditskiy, Aleksey; Peng, Hsin-Chieh Chemical Reviews, Vol. 116, Issue 18 https://doi.org/10.1021/acs.chemrev.6b00211	journal	July 2016
Amorphous versus Crystalline in Water Oxidation Catalysis: A Case Study of NiFe Alloy Cai, Weizheng; Chen, Rong; Yang, Hongbin Nano Letters, Vol. 20, Issue 6 https://doi.org/10.1021/acs.nanolett.0c00840	journal	May 2020
Double-Network Nanostructured Hydrogel-Derived Ultrafine Sn–Fe Alloy in Three-Dimensional Carbon Framework for Enhanced Lithium Storage Shi, Hongxia; Fang, Zhiwei; Zhang, Xiao Nano Letters, Vol. 18, Issue 5 https://doi.org/10.1021/acs.nanolett.8b00898	journal	April 2018
Inorganic Gel-Derived Metallic Frameworks Enabling High-Performance Silicon Anodes Zhang, Anping; Fang, Zhiwei; Tang, Yawen Nano Letters, Vol. 19, Issue 9 https://doi.org/10.1021/acs.nanolett.9b02429	journal	August 2019
Two-Dimensional Mosaic Bismuth Nanosheets for Highly Selective Ambient Electrocatalytic Nitrogen Reduction Li, Laiquan; Tang, Cheng; Xia, Bingquan ACS Catalysis, Vol. 9, Issue 4 https://doi.org/10.1021/acscatal.9b00366	journal	February 2019
Diverse Polymeric Carbon Nitride-Based Semiconductors for Photocatalysis and Variations Fang, Yuanxing; Fu, Xianzhi; Wang, Xinchen ACS Materials Letters, Vol. 2, Issue 8 https://doi.org/10.1021/acsmaterialslett.0c00215	journal	June 2020
Inorganic Cyanogels and Their Derivatives for Electrochemical Energy Storage and Conversion Fang, Zhiwei; Zhang, Anping; Wu, Ping ACS Materials Letters, Vol. 1, Issue 1 https://doi.org/10.1021/acsmaterialslett.9b00125	journal	May 2019
Cyanogel-Enabled Homogeneous Sb–Ni–C Ternary Framework Electrodes for Enhanced Sodium Storage Wu, Ping; Zhang, Anping; Peng, Lele ACS Nano, Vol. 12, Issue 1 https://doi.org/10.1021/acsnano.7b07985	journal	January 2018
Rational Design of Rhodium–Iridium Alloy Nanoparticles as Highly Active Catalysts for Acidic Oxygen Evolution Guo, Hongyu; Fang, Zhiwei; Li, Hao ACS Nano, Vol. 13, Issue 11 https://doi.org/10.1021/acsnano.9b06244	journal	October 2019
Hybrid Organic–Inorganic Gel Electrocatalyst for Stable Acidic Water Oxidation Fang, Zhiwei; Wu, Ping; Yu, Kang ACS Nano, Vol. 13, Issue 12 https://doi.org/10.1021/acsnano.9b07826	journal	November 2019
Introduction to Metal–Organic Frameworks Zhou, Hong-Cai; Long, Jeffrey R.; Yaghi, Omar M. Chemical Reviews, Vol. 112, Issue 2, p. 673-674 https://doi.org/10.1021/cr300014x	journal	September 2011
A Robust and Biocompatible Bismuth Ellagate MOF Synthesized Under Green Ambient Conditions Grape, Erik Svensson; Flores, J. Gabriel; Hidalgo, Tania Journal of the American Chemical Society, Vol. 142, Issue 39 https://doi.org/10.1021/jacs.0c07525	journal	September 2020
Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li ⁺ Incorporation Strategy Chen, Gao-Feng; Cao, Xinrui; Wu, Shunqing Journal of the American Chemical Society, Vol. 139, Issue 29 https://doi.org/10.1021/jacs.7b04393	journal	July 2017
Electrochemical Reduction of N ₂ into NH ₃ by Donor–Acceptor Couples of Ni and Au Nanoparticles with a 67.8% Faradaic Efficiency Xue, Zhong-Hua; Zhang, Shi-Nan; Lin, Yun-Xiao Journal of the American Chemical Society, Vol. 141, Issue 38 https://doi.org/10.1021/jacs.9b07963	journal	September 2019
Ultrathin bismuth nanosheets from in situ topotactic transformation for selective electrocatalytic CO2 reduction to formate Han, Na; Wang, Yu; Yang, Hui Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03712-z	journal	April 2018
Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation Liu, Sisi; Wang, Mengfan; Qian, Tao Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11846-x	journal	August 2019
Promoting nitrogen electroreduction to ammonia with bismuth nanocrystals and potassium cations in water Hao, Yu-Chen; Guo, Yu; Chen, Li-Wei Nature Catalysis, Vol. 2, Issue 5 https://doi.org/10.1038/s41929-019-0241-7	journal	March 2019
Challenges and prospects in the catalysis of electroreduction of nitrogen to ammonia Suryanto, Bryan H. R.; Du, Hoang-Long; Wang, Dabin Nature Catalysis, Vol. 2, Issue 4 https://doi.org/10.1038/s41929-019-0252-4	journal	March 2019
Challenges in reduction of dinitrogen by proton and electron transfer van der Ham, Cornelis J. M.; Koper, Marc T. M.; Hetterscheid, Dennis G. H. Chem. Soc. Rev., Vol. 43, Issue 15 https://doi.org/10.1039/C4CS00085D	journal	January 2014
Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH ₃ ) under ambient conditions Guo, Chunxian; Ran, Jingrun; Vasileff, Anthony Energy & Environmental Science, Vol. 11, Issue 1 https://doi.org/10.1039/C7EE02220D	journal	January 2018
Electrochemical nitrogen fixation and utilization: theories, advanced catalyst materials and system design Guo, Wenhan; Zhang, Kexin; Liang, Zibin Chemical Society Reviews, Vol. 48, Issue 24 https://doi.org/10.1039/C9CS00159J	journal	January 2019
Understanding the boosted sodium storage behavior of a nanoporous bismuth-nickel anode using operando X-ray diffraction and density functional theory calculations Gao, Hui; Song, Lin; Niu, Jiazheng Journal of Materials Chemistry A, Vol. 7, Issue 22 https://doi.org/10.1039/C9TA03810H	journal	January 2019
Multi-yolk–shell bismuth@porous carbon as a highly efficient electrocatalyst for artificial N ₂ fixation under ambient conditions Qiu, Yu; Zhao, Sen; Qin, Mingxin Inorganic Chemistry Frontiers, Vol. 7, Issue 10 https://doi.org/10.1039/D0QI00153H	journal	January 2020
Alternative catalytic materials: carbides, nitrides, phosphides and amorphous boron alloys Alexander, Anne-Marie; Hargreaves, Justin S. J. Chemical Society Reviews, Vol. 39, Issue 11 https://doi.org/10.1039/b916787k	journal	January 2010
Favoring the unfavored: Selective electrochemical nitrogen fixation using a reticular chemistry approach Lee, Hiang Kwee; Koh, Charlynn Sher Lin; Lee, Yih Hong Science Advances, Vol. 4, Issue 3 https://doi.org/10.1126/sciadv.aar3208	journal	March 2018
Ammonia synthesis by N2 and steam electrolysis in molten hydroxide suspensions of nanoscale Fe2O3 Licht, S.; Cui, B.; Wang, B. Science, Vol. 345, Issue 6197 https://doi.org/10.1126/science.1254234	journal	August 2014
Carbothermal shock synthesis of high-entropy-alloy nanoparticles Yao, Yonggang; Huang, Zhennan; Xie, Pengfei Science, Vol. 359, Issue 6383 https://doi.org/10.1126/science.aan5412	journal	March 2018

Similar Records

Gel-Derived Amorphous Bismuth–Nickel Alloy Promotes Electrocatalytic Nitrogen Fixation via Optimizing Nitrogen Adsorption and Activation

Journal Article · Sun Nov 15 19:00:00 EST 2020 · Angewandte Chemie (International Edition) · OSTI ID:1774921

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Journal Article · Thu Jan 17 19:00:00 EST 2019 · Angewandte Chemie · OSTI ID:1786172

Gel‐Derived Amorphous Bismuth–Nickel Alloy Promotes Electrocatalytic Nitrogen Fixation via Optimizing Nitrogen Adsorption and Activation

Citation Formats

References (49)

Similar Records

Related Subjects