Strongly Coupled Ag/Sn-SnO2 Nanosheets Toward CO2 Electroreduction to Pure HCOOH Solutions at Ampere-Level CurrentOACSTPCD
Strongly Coupled Ag/Sn-SnO2 Nanosheets Toward CO2 Electroreduction to Pure HCOOH Solutions at Ampere-Level Current
Electrocatalytic reduction of CO2 converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO2 grains,designated as Ag/Sn-SnO2 nanosheets(NSs),which possess optimized electronic structure,high electri-cal conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO2-to-formate conversion with near-unity faradaic efficiency(＞90％),ultrahigh partial current density(2,000 mA cm-2),and superior long-term stability(200 mA cm-2,200 h),surpassing the reported catalysts of CO2 electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical cal-culations revealed that electron-enriched Sn sites on Ag/Sn-SnO2 NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO2 NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce～0.12 M pure HCOOH solution at 100 mA cm-2 over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO2.
Min Zhang;Aihui Cao;Yucui Xiang;Chaogang Ban;Guang Han;Junjie Ding;Li-Yong Gan;Xiaoyuan Zhou
College of Physics and Center of Quantum Materials and Devices,Chongqing University,Chongqing 401331,People's Republic of ChinaState Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences(CAS),Fuzhou 350002,People's Republic of ChinaCollege of Materials Science and Engineering,Chongqing University,Chongqing 400044,People's Republic of China||Institute of New Energy Storage Materials and Equipment,Chongqing 401135,People's Republic of ChinaCollege of Physics and Center of Quantum Materials and Devices,Chongqing University,Chongqing 401331,People's Republic of China||Institute of New Energy Storage Materials and Equipment,Chongqing 401135,People's Republic of China||State Key Laboratory of Coal Mine Disaster Dynamics and Control,Chongqing University,Chongqing 400044,People's Republic of China
Electrochemical CO2 reductionCoupled Ag/Sn-SnO2 nanosheetsElectronic structurePorous solid electrolytePure HCOOH solution
《纳微快报（英文）》 2024 (003)
212-226 / 15
This work was financially supported from the National Science Fund for Distinguished Young Scholars(Grant No.52125103),the National Natural Science Foundation of China(Grant Nos.52301232,52071041,12074048,and 12147102),and China Postdoctoral Science Foundation(Grant No.2022M720552).The authors would like to thank the Analytical and Testing Center of Chongqing University for the assistance with the sample characterization.
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