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Vol. 16 (2024)

Strongly Coupled Ag/Sn–SnO2 Nanosheets Toward CO2 Electroreduction to Pure HCOOH Solutions at Ampere-Level Current

https://doi.org/10.1007/s40820-023-01264-6
Min Zhang
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, People’s Republic of China
Aihui Cao
State 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 China
Yucui Xiang
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, People’s Republic of China
Chaogang Ban
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, People’s Republic of China
Guang Han
College of Materials Science and Engineering, Chongqing University, Chongqing 400044, People’s Republic of China
Junjie Ding
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, People’s Republic of China
Li‑Yong Gan
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, People’s Republic of China
Xiaoyuan Zhou
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, People’s Republic of China

Corresponding Author: Xiaoyuan Zhou

xiaoyuan2013@cqu.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 50

Abstract

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 electrical 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 calculations 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.


Highlights:
1 The strongly coupled Ag/Sn–SnO2 nanosheets (NSs) were prepared via a versatile electrochemical template strategy, and the generated electron-enriched Sn sites promote the formation of *OCHO and alleviate the energy barriers of *OCHO to *HCOOH.
2 Ag/Sn–SnO2 NSs afford a superior activity toward CO2 electroreduction with current densities up to 2000 mA cm‒2 and near-unity selectivity for formate production.
3 Ag/Sn–SnO2 NSs as the cathode in a membrane electrode assembly with porous solid electrolyte reactor enable the direct production of ~ 0.12 M pure HCOOH solution for 200 h.

Keywords

Electrochemical CO2 reduction Coupled Ag/Sn–SnO2 nanosheets Electronic structure Porous solid electrolyte Pure HCOOH solution
Zhang, Min, Aihui Cao, Yucui Xiang, Chaogang Ban, Guang Han, Junjie Ding, Li‑Yong Gan, and Xiaoyuan Zhou. 2023. “Strongly Coupled Ag/Sn–SnO2 Nanosheets Toward CO2 Electroreduction to Pure HCOOH Solutions at Ampere-Level Current”. Nano-Micro Letters 16 (December):50. https://doi.org/10.1007/s40820-023-01264-6.
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