Synergistic Cr 2 O 3 @Ag Heterostructure Enhanced Electrocatalytic CO 2 Reduction to CO

Fu, Huai Qin; Liu, Junxian; Bedford, Nicholas M.; Wang, Yun; Sun, Ji Wei; Zou, Yu; Dong, Mengyang; Wright, Joshua; Diao, Hui; Liu, Porun; Yang, Hua Gui; Zhao, Huijun

doi:10.1002/adma.202202854

Title: Synergistic Cr ₂ O ₃ @Ag Heterostructure Enhanced Electrocatalytic CO ₂ Reduction to CO

Journal Article · Fri Jun 10 00:00:00 EDT 2022 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202202854· OSTI ID:1872150

Fu, Huai Qin ^[1]; Liu, Junxian ^[1]; Bedford, Nicholas M. ^[2]; Wang, Yun ^[1]; Sun, Ji Wei ^[3]; Zou, Yu ^[1]; Dong, Mengyang ^[1]; Wright, Joshua ^[4]; Diao, Hui ^[5]; Liu, Porun ^[1]; Yang, Hua Gui ^[3];

^[1]

Centre for Catalysis and Clean Energy Gold Coast Campus Griffith University Queensland 4222 Australia
School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia
Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai 200237 China
Department of Physics Illinois Institute of Technology Chicago IL 60616 USA
The Centre for Microscopy and Microanalysis The University of Queensland St Lucia QLD 4072 Australia

Abstract The electrocatalytic CO ₂ RR to produce value‐added chemicals and fuels has been recognized as a promising means to reduce the reliance on fossil resources; it is, however, hindered due to the lack of high‐performance electrocatalysts. The effectiveness of sculpturing metal/metal oxides (MMO) heterostructures to enhance electrocatalytic performance toward CO ₂ RR has been well documented, nonetheless, the precise synergistic mechanism of MMO remains elusive. Herein, an in operando electrochemically synthesized Cr ₂ O ₃ –Ag heterostructure electrocatalyst (Cr ₂ O ₃ @Ag) is reported for efficient electrocatalytic reduction of CO ₂ to CO. The obtained Cr ₂ O ₃ @Ag can readily achieve a superb FE _CO of 99.6% at −0.8 V (vs RHE) with a high J _CO of 19.0 mA cm ⁻² . These studies also confirm that the operando synthesized Cr ₂ O ₃ @Ag possesses high operational stability. Notably, operando Raman spectroscopy studies reveal that the markedly enhanced performance is attributable to the synergistic Cr ₂ O ₃ –Ag heterostructure induced stabilization of CO ₂ ^•− /*COOH intermediates. DFT calculations unveil that the metallic‐Ag‐catalyzed CO ₂ reduction to CO requires a 1.45 eV energy input to proceed, which is 0.93 eV higher than that of the MMO‐structured Cr ₂ O ₃ @Ag. The exemplified approaches in this work would be adoptable for design and development of high‐performance electrocatalysts for other important reactions.

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Sponsoring Organization:: USDOE

OSTI ID:: 1872150

Alternate ID(s):: OSTI ID: 1872151

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Vol. 34 Journal Issue: 29; ISSN 0935-9648

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

Country of Publication:: Germany

Language:: English

References (59)

Sn(II) oxy-hydroxides as potential adsorbents for Cr(VI)-uptake from drinking water: An X-ray absorption study Pinakidou, Fani; Kaprara, Efthimia; Katsikini, Maria Science of The Total Environment, Vol. 551-552 https://doi.org/10.1016/j.scitotenv.2016.01.208	journal	May 2016
Far-infrared spectra of amino acids Matei, Adriana; Drichko, Natalia; Gompf, Bruno Chemical Physics, Vol. 316, Issue 1-3 https://doi.org/10.1016/j.chemphys.2005.04.033	journal	September 2005
Electroreduction of CO ₂ to Formate on a Copper-Based Electrocatalyst at High Pressures with High Energy Conversion Efficiency Li, Jiachen; Kuang, Yun; Meng, Yongtao Journal of the American Chemical Society, Vol. 142, Issue 16 https://doi.org/10.1021/jacs.0c00122	journal	April 2020
Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation Wang, Xue; Wang, Ziyun; García de Arquer, F. Pelayo Nature Energy, Vol. 5, Issue 6 https://doi.org/10.1038/s41560-020-0607-8	journal	May 2020
Unlocking Bifunctional Electrocatalytic Activity for CO ₂ Reduction Reaction by Win-Win Metal–Oxide Cooperation Cai, Zhao; Wu, Yueshen; Wu, Zishan ACS Energy Letters, Vol. 3, Issue 11 https://doi.org/10.1021/acsenergylett.8b01767	journal	October 2018
Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO ₂ Electroreduction to Formate Li, Zhongjian; Cao, Ang; Zheng, Qiang Advanced Materials, Vol. 33, Issue 2 https://doi.org/10.1002/adma.202005113	journal	November 2020
Aqueous-phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy Michailoudi, Georgia; Lin, Jack J.; Yuzawa, Hayato Atmospheric Chemistry and Physics, Vol. 21, Issue 4 https://doi.org/10.5194/acp-21-2881-2021	journal	January 2021
Unraveling Structure Sensitivity in CO ₂ Electroreduction to Near-Unity CO on Silver Nanocubes Liu, Subiao; Sun, Chong; Xiao, Jing ACS Catalysis, Vol. 10, Issue 5 https://doi.org/10.1021/acscatal.9b03883	journal	February 2020
Enhancing CO ₂ Electroreduction with the Metal–Oxide Interface Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen Journal of the American Chemical Society, Vol. 139, Issue 16 https://doi.org/10.1021/jacs.7b00102	journal	April 2017
Densely Packed, Ultra Small SnO Nanoparticles for Enhanced Activity and Selectivity in Electrochemical CO ₂ Reduction Gu, Jun; Héroguel, Florent; Luterbacher, Jeremy Angewandte Chemie, Vol. 130, Issue 11 https://doi.org/10.1002/ange.201713003	journal	February 2018
Assignments of the vibrational frequencies of glycine Tsuboi, Masamichi; Onishi, Takaharu; Nakagawa, Ichiro Spectrochimica Acta, Vol. 12, Issue 2-3 https://doi.org/10.1016/0371-1951(58)80041-7	journal	September 1958
“Two Ships in a Bottle” Design for Zn–Ag–O Catalyst Enabling Selective and Long-Lasting CO ₂ Electroreduction Zhang, Zhen; Wen, Guobin; Luo, Dan Journal of the American Chemical Society, Vol. 143, Issue 18 https://doi.org/10.1021/jacs.0c12418	journal	April 2021
Highly Selective CO ₂ Electroreduction to CH ₄ by In Situ Generated Cu ₂ O Single‐Type Sites on a Conductive MOF: Stabilizing Key Intermediates with Hydrogen Bonding Yi, Jun‐Dong; Xie, Ruikuan; Xie, Zai‐Lai Angewandte Chemie International Edition, Vol. 59, Issue 52 https://doi.org/10.1002/anie.202010601	journal	October 2020
Interface Engineering of Silver-Based Heterostructures for CO ₂ Reduction Reaction Yuan, Xiaolei; Wu, Yueshen; Jiang, Bei ACS Applied Materials & Interfaces, Vol. 12, Issue 50 https://doi.org/10.1021/acsami.0c19031	journal	December 2020
Fabrication of AgBr/Ag2CrO4 composites for enhanced visible-light photocatalytic activity Zhu, Lifang; Huang, Daiqin; Ma, Jianfeng Ceramics International, Vol. 41, Issue 9 https://doi.org/10.1016/j.ceramint.2015.05.118	journal	November 2015
Strongly Coupled Cobalt Diselenide Monolayers for Selective Electrocatalytic Oxygen Reduction to H ₂ O ₂ under Acidic Conditions Zhang, Xiao‐Long; Su, Xiaozhi; Zheng, Ya‐Rong Angewandte Chemie International Edition, Vol. 60, Issue 52 https://doi.org/10.1002/anie.202111075	journal	October 2021
Adsorption of CO3 on a silver electrode in Na2CO3 solution studied by SERS Sasaki, Y.; Iwasaki, N.; Nishina, Y. Surface Science, Vol. 198, Issue 3 https://doi.org/10.1016/0039-6028(88)90383-4	journal	January 1988
Efficient and Robust Carbon Dioxide Electroreduction Enabled by Atomically Dispersed Sn δ + Sites Zu, Xiaolong; Li, Xiaodong; Liu, Wei Advanced Materials, Vol. 31, Issue 15 https://doi.org/10.1002/adma.201808135	journal	February 2019
Revised pourbaix diagrams for chromium at 25–300 °C Beverskog, B.; Puigdomenech, I. Corrosion Science, Vol. 39, Issue 1 https://doi.org/10.1016/S0010-938X(97)89244-X	journal	January 1997
Electrocatalytic Reduction of CO ₂ to CO over Ag(110) and Cu(211) Modeled by Grand-Canonical Density Functional Theory Alsunni, Yousef A.; Alherz, Abdulaziz W.; Musgrave, Charles B. The Journal of Physical Chemistry C, Vol. 125, Issue 43 https://doi.org/10.1021/acs.jpcc.1c07484	journal	October 2021
In-situ solid-state synthesis and regulation of Ag2O/Ag2CO3 heterojunctions with promoted visible-light driven photocatalytic decomposition for organic pollutant Hu, Jindou; Xu, Hui; Wang, Shiqiang Separation and Purification Technology, Vol. 226 https://doi.org/10.1016/j.seppur.2019.05.080	journal	November 2019
Ag2CrO4 for photocatalytic applications: High performance of crystals designed by autogenous pressure Miclau, Marinela; Kumar, Sanjay; Ursu, Daniel Materials Characterization, Vol. 158 https://doi.org/10.1016/j.matchar.2019.109970	journal	December 2019
Electroreduction of Carbon Dioxide Driven by the Intrinsic Defects in the Carbon Plane of a Single Fe–N ₄ Site Ni, Wenpeng; Liu, Zhixiao; Zhang, Yan Advanced Materials, Vol. 33, Issue 1 https://doi.org/10.1002/adma.202003238	journal	November 2020
A micro-Raman spectroscopic study of Cr(OH) ₃ and Cr ₂ O ₃ nanoparticles obtained by the hydrothermal method: A micro-Raman spectroscopic study of Cr(OH) ₃ and Cr ₂ O ₃ nanoparticles Gomes, Adriano S. O.; Yaghini, Negin; Martinelli, Anna Journal of Raman Spectroscopy, Vol. 48, Issue 10 https://doi.org/10.1002/jrs.5198	journal	August 2017
High-pressure study of Cr2O3 obtained by high-temperature oxidation by X-ray diffraction and Raman spectroscopy Mougin, J.; Le Bihan, T.; Lucazeau, G. Journal of Physics and Chemistry of Solids, Vol. 62, Issue 3 https://doi.org/10.1016/S0022-3697(00)00215-8	journal	March 2001
Defective Bimetallic Selenides for Selective CO ₂ Electroreduction to CO Wang, Jiajun; Zheng, Xuerong; Wang, Guangjin Advanced Materials, Vol. 34, Issue 3 https://doi.org/10.1002/adma.202106354	journal	December 2021
Synergistic effects in silver–indium electrocatalysts for carbon dioxide reduction Larrazábal, Gastón O.; Martín, Antonio J.; Mitchell, Sharon Journal of Catalysis, Vol. 343 https://doi.org/10.1016/j.jcat.2015.12.014	journal	November 2016
Tunable Cu Enrichment Enables Designer Syngas Electrosynthesis from CO ₂ Ross, Michael B.; Dinh, Cao Thang; Li, Yifan Journal of the American Chemical Society, Vol. 139, Issue 27 https://doi.org/10.1021/jacs.7b04892	journal	June 2017
Understanding the electric and nonelectric field components of the cation effect on the electrochemical CO reduction reaction Malkani, A. S.; Li, J.; Oliveira, N. J. Science Advances, Vol. 6, Issue 45 https://doi.org/10.1126/sciadv.abd2569	journal	November 2020
Raman Spectroscopy and Single-Crystal High-Temperature Investigations of Bentorite, Ca6Cr2(SO4)3(OH)12·26H2O Juroszek, Rafał; Krüger, Biljana; Galuskina, Irina Minerals, Vol. 10, Issue 1 https://doi.org/10.3390/min10010038	journal	December 2019
Computational Screening of Near-Surface Alloys for CO ₂ Electroreduction Zhao, Zhonglong; Lu, Gang ACS Catalysis, Vol. 8, Issue 5 https://doi.org/10.1021/acscatal.7b03705	journal	March 2018
Surface and Interface Engineering in Copper-Based Bimetallic Materials for Selective CO2 Electroreduction Vasileff, Anthony; Xu, Chaochen; Jiao, Yan Chem, Vol. 4, Issue 8 https://doi.org/10.1016/j.chempr.2018.05.001	journal	August 2018
Heterostructured Catalysts for Electrocatalytic and Photocatalytic Carbon Dioxide Reduction Prabhu, P.; Jose, Vishal; Lee, Jong‐Min Advanced Functional Materials, Vol. 30, Issue 24 https://doi.org/10.1002/adfm.201910768	journal	April 2020
Metallic tin quantum sheets confined in graphene toward high-efficiency carbon dioxide electroreduction Lei, Fengcai; Liu, Wei; Sun, Yongfu Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12697	journal	September 2016
Non-destructive Rapid Analysis Discriminating between Chromium(VI) and Chromium(III) Oxides in Electrical and Electronic Equipment Using Raman Spectroscopy Kikuchi, Sonoko; Kawauchi, Kazuteru; Kurosawa, Masaru Analytical Sciences, Vol. 21, Issue 3 https://doi.org/10.2116/analsci.21.197	journal	January 2005
Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction Tan, Ying Chuan; Lee, Kelvin Berm; Song, Hakhyeon Joule, Vol. 4, Issue 5 https://doi.org/10.1016/j.joule.2020.03.013	journal	May 2020
Silver Single‐Atom Catalyst for Efficient Electrochemical CO ₂ Reduction Synthesized from Thermal Transformation and Surface Reconstruction Zhang, Ningqiang; Zhang, Xinxin; Tao, Lei Angewandte Chemie International Edition, Vol. 60, Issue 11 https://doi.org/10.1002/anie.202014718	journal	January 2021
Designing a Zn–Ag Catalyst Matrix and Electrolyzer System for CO ₂ Conversion to CO and Beyond Lamaison, Sarah; Wakerley, David; Kracke, Frauke Advanced Materials, Vol. 34, Issue 1 https://doi.org/10.1002/adma.202103963	journal	October 2021
Oxygen Functionalities Evolution in Thermally Treated Graphene Oxide Featured by EELS and DFT Calculations D’Angelo, D.; Bongiorno, C.; Amato, M. The Journal of Physical Chemistry C, Vol. 121, Issue 9 https://doi.org/10.1021/acs.jpcc.7b00239	journal	February 2017
Electronic and crystal structures of $({Na}_{1 - x} {Ca}_{x}) {Cr}_{2} O_{4}$ with anomalous colossal magnetoresistance Yamaoka, Hitoshi; Schwier, Eike F.; Yamamoto, Yoshiya Physical Review B, Vol. 102, Issue 23 https://doi.org/10.1103/PhysRevB.102.235150	journal	December 2020
A review of non-noble metal-based electrocatalysts for CO2 electroreduction Wang, Jia-Jun; Li, Xiao-Peng; Cui, Bing-Feng Rare Metals, Vol. 40, Issue 11 https://doi.org/10.1007/s12598-021-01736-x	journal	May 2021
Transition of chromium oxyhydroxide nanomaterials to chromium oxide: a hot-stage Raman spectroscopic study Yang, Jing Jeanne; Martens, Wayde N.; Frost, Ray L. Journal of Raman Spectroscopy, Vol. 42, Issue 5 https://doi.org/10.1002/jrs.2773	journal	August 2010
Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration Liu, Min; Pang, Yuanjie; Zhang, Bo Nature, Vol. 537, Issue 7620 https://doi.org/10.1038/nature19060	journal	August 2016
Ni nanoparticle-decorated-MnO ₂ nanodendrites as highly selective and efficient catalysts for CO ₂ electroreduction He, Xu-Jun; Feng, Jin-Xian; Ren, Qian Journal of Materials Chemistry A, Vol. 6, Issue 40 https://doi.org/10.1039/C8TA07687A	journal	January 2018
Boosting Tunable Syngas Formation via Electrochemical CO ₂ Reduction on Cu/In ₂ O ₃ Core/Shell Nanoparticles Xie, Huan; Chen, Shaoqing; Ma, Feng ACS Applied Materials & Interfaces, Vol. 10, Issue 43 https://doi.org/10.1021/acsami.8b12747	journal	October 2018
Electrode Materials Engineering in Electrocatalytic CO ₂ Reduction: Energy Input and Conversion Efficiency Song, Rong‐Bin; Zhu, Wenlei; Fu, Jiaju Advanced Materials https://doi.org/10.1002/adma.201903796	journal	October 2019
Combined DRS–RS–EXAFS–XANES–TPR study of supported chromium catalysts Weckhuysen, Bert M.; Schoonheydt, Robert A.; Jehng, Jih-Mirn J. Chem. Soc., Faraday Trans., Vol. 91, Issue 18 https://doi.org/10.1039/FT9959103245	journal	January 1995
Heterogeneous Single‐Atom Catalysts for Electrochemical CO ₂ Reduction Reaction Li, Minhan; Wang, Haifeng; Luo, Wei Advanced Materials, Vol. 32, Issue 34 https://doi.org/10.1002/adma.202001848	journal	July 2020
Micro and conventional XAFS study of incinerated Cr-rich tannery sludge Pinakidou, F.; Katsikini, M.; Varitis, S. Journal of Physics: Conference Series, Vol. 712 https://doi.org/10.1088/1742-6596/712/1/012099	journal	May 2016
Carbon Solving Carbon's Problems: Recent Progress of Nanostructured Carbon-Based Catalysts for the Electrochemical Reduction of CO ₂ Vasileff, Anthony; Zheng, Yao; Qiao, Shi Zhang Advanced Energy Materials, Vol. 7, Issue 21 https://doi.org/10.1002/aenm.201700759	journal	July 2017
The role of in situ generated morphological motifs and Cu(i) species in C2+ product selectivity during CO2 pulsed electroreduction Arán-Ais, Rosa M.; Scholten, Fabian; Kunze, Sebastian Nature Energy, Vol. 5, Issue 4 https://doi.org/10.1038/s41560-020-0594-9	journal	March 2020
Silver Supported on Titania as an Active Catalyst for Electrochemical Carbon Dioxide Reduction Ma , Sichao; Lan , Yangchun; Perez, Gaby M. J. ChemSusChem, Vol. 7, Issue 3 https://doi.org/10.1002/cssc.201300934	journal	January 2014
Shape-Dependent Electrocatalytic Reduction of CO ₂ to CO on Triangular Silver Nanoplates Liu, Subiao; Tao, Hongbiao; Zeng, Li Journal of the American Chemical Society, Vol. 139, Issue 6 https://doi.org/10.1021/jacs.6b12103	journal	February 2017
Metal–Organic Framework‐Based Electrocatalysts for CO ₂ Reduction Shah, Syed Shoaib Ahmad; Najam, Tayyaba; Wen, Ming Small Structures, Vol. 3, Issue 5 https://doi.org/10.1002/sstr.202100090	journal	September 2021
Probing the Reaction Mechanism of CO ₂ Electroreduction over Ag Films via Operando Infrared Spectroscopy Firet, Nienke J.; Smith, Wilson A. ACS Catalysis, Vol. 7, Issue 1 https://doi.org/10.1021/acscatal.6b02382	journal	December 2016
Quantifying Electrocatalytic Reduction of CO2 on Twin Boundaries Hu, Feng; Abeyweera, Sasitha C.; Yu, Jie Chem, Vol. 6, Issue 11 https://doi.org/10.1016/j.chempr.2020.07.026	journal	November 2020
Achieving Selective and Efficient Electrocatalytic Activity for CO ₂ Reduction Using Immobilized Silver Nanoparticles Kim, Cheonghee; Jeon, Hyo Sang; Eom, Taedaehyeong Journal of the American Chemical Society, Vol. 137, Issue 43 https://doi.org/10.1021/jacs.5b06568	journal	October 2015
Ultrathin Co ₃ O ₄ Layers Realizing Optimized CO ₂ Electroreduction to Formate Gao, Shan; Jiao, Xingchen; Sun, Zhongti Angewandte Chemie International Edition, Vol. 55, Issue 2 https://doi.org/10.1002/anie.201509800	journal	November 2015
A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels Qiao, Jinli; Liu, Yuyu; Hong, Feng Chem. Soc. Rev., Vol. 43, Issue 2 https://doi.org/10.1039/C3CS60323G	journal	January 2014

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