Atom vacancies induced electron-rich surface of ultrathin Bi nanosheet for efficient electrochemical CO2 reduction

Zhao, Mengya; Gu, Yaliu; Gao, Weicheng; Cui, Peixin; Tang, Huang; Wei, Xinying; Zhu, Heng; Li, Guoqiang; Yan, Shicheng; Zhang, Xiuyun; Zou, Zhigang

doi:10.1016/j.apcatb.2020.118625

Cited by 122 publications

(51 citation statements)

References 44 publications

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“…[23] In addition, the electron states of both the Opand Sn p, do rbitals are upshift away from the fermi level after the formation of the heterojunction of CuS@SnO 2 and Cu 2 O@SnO 2 ,w hich also indicates astrongest binding force the between HCOO* and the heterojunction surface. [24] Moreover,t he upshift electron states of Oporbitals means that the Oatom of HCOO* which absorbed in the heterojunction surface increase the antibonding states compared to that of SnO 2 . [17e,25] In other word, HCOO* absorbed in the heterojunction surface allow H* to accessibly adsorb and react with HCOO*.…”

Section: Methodsmentioning

confidence: 99%

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

Wang

Yang

et al. 2021

Angew Chem Int Ed

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Bimetallic sulfides are expected to realize efficient CO 2 electroreduction into formate over aw ide potential window,however,they will undergo in situ structural evolution under the reaction conditions.T herefore,c larifying the structural evolution process,t he real active site and the catalytic mechanism is significant. Here,taking Cu 2 SnS 3 as an example, we unveiled that Cu 2 SnS 3 occurred self-adapted phase separation towardf orming the stable SnO 2 @CuS and SnO 2 @Cu 2 O heterojunction during the electrochemical process.C alculations illustrated that the strongly coupled interfaces as real active sites driven the electron self-flow from Sn 4+ to Cu + , therebypromoting the delocalized Sn sites to combine HCOO* with H*. Cu 2 SnS 3 nanosheets achieve over 83.4 %f ormate selectivity in awide potential range from À0.6 VtoÀ1.1 V. Our findings provide insight into the structural evolution process and performance-enhanced origin of ternary sulfides under the CO 2 electroreduction.

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Section: Methodsmentioning

confidence: 99%

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

Wang

Yang

et al. 2021

Angew Chem Int Ed

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“…Chemie Forschungsartikel 23126 www.angewandte.de the electron states of both the Opand Sn p, do rbitals are upshift away from the fermi level after the formation of the heterojunction of CuS@SnO 2 and Cu 2 O@SnO 2 ,w hich also indicates astrongest binding force the between HCOO* and the heterojunction surface. [24] Moreover,t he upshift electron states of Oporbitals means that the Oatom of HCOO* which absorbed in the heterojunction surface increase the antibonding states compared to that of SnO 2 . [17e,25] In other word, HCOO* absorbed in the heterojunction surface allow H* to accessibly adsorb and react with HCOO*.…”

Section: Methodsmentioning

confidence: 99%

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

Wang

Yang

et al. 2021

Angewandte Chemie

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Bimetallic sulfides are expected to realize efficient CO2 electroreduction into formate over a wide potential window, however, they will undergo in situ structural evolution under the reaction conditions. Therefore, clarifying the structural evolution process, the real active site and the catalytic mechanism is significant. Here, taking Cu2SnS3 as an example, we unveiled that Cu2SnS3 occurred self‐adapted phase separation toward forming the stable SnO2@CuS and SnO2@Cu2O heterojunction during the electrochemical process. Calculations illustrated that the strongly coupled interfaces as real active sites driven the electron self‐flow from Sn4+ to Cu+, thereby promoting the delocalized Sn sites to combine HCOO* with H*. Cu2SnS3 nanosheets achieve over 83.4 % formate selectivity in a wide potential range from −0.6 V to −1.1 V. Our findings provide insight into the structural evolution process and performance‐enhanced origin of ternary sulfides under the CO2 electroreduction.

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“…[11] The latter aims to adjust the adsorption of intermediates and smooth reaction pathways by regulating the electronic structure. [12] Up to date, reported researches for modifying the electronic structure have provided effective ways including introducing vacancies [13] and grain boundaries. [14] Theoretical studies reveal that introducing p-block atoms is effective on breaking linear scaling relations for the Gibbs free energy of *COOH and *OCHO which are the intermediates for CO and formate, respectively.…”

Section: Introductionmentioning

confidence: 99%

Boron Dopant Induced Electron‐Rich Bismuth for Electrochemical CO₂ Reduction with High Solar Energy Conversion Efficiency

Chen

Zhou

et al. 2021

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Electrochemical CO 2 reduction to formate offers a mild and feasible pathway for the utilization of CO 2 , and bismuth is a promising metal for its unique hydrogen evolution reaction inhibition. Reported works of Bi-based electrodes generally exhibit high selectivity while suffering from relatively narrow working potential range. From the perspective of electronic modification engineering, B-doped Bi is prepared by a facile chemical reduction method in this work. With B dopant, above 90% Faradaic efficiency for formate over a broad window of working potential of −0.6 to −1.2 V (vs. reversible hydrogen electrode) is achieved. In situ Raman spectroscopy, X-ray adsorption spectroscopy, and computational analysis demonstrate that the B dopant induces the formation of electron-rich bismuth, which is in favor of the formation of formate by fine-tuning the adsorption energy of *OCHO. Moreover, full-cell electrolysis system coupled with photovoltaic device is constructed and achieves the solar-to-formate conversion efficiency as high as 11.8%.

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Atom vacancies induced electron-rich surface of ultrathin Bi nanosheet for efficient electrochemical CO2 reduction

Cited by 122 publications

References 44 publications

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

Boron Dopant Induced Electron‐Rich Bismuth for Electrochemical CO₂ Reduction with High Solar Energy Conversion Efficiency

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Atom vacancies induced electron-rich surface of ultrathin Bi nanosheet for efficient electrochemical CO2 reduction

Cited by 122 publications

References 44 publications

In Situ Phase Separation into Coupled Interfaces for Promoting CO2 Electroreduction to Formate over a Wide Potential Window

In Situ Phase Separation into Coupled Interfaces for Promoting CO2 Electroreduction to Formate over a Wide Potential Window

In Situ Phase Separation into Coupled Interfaces for Promoting CO2 Electroreduction to Formate over a Wide Potential Window

Boron Dopant Induced Electron‐Rich Bismuth for Electrochemical CO2 Reduction with High Solar Energy Conversion Efficiency

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Product

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In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

In Situ Phase Separation into Coupled Interfaces for Promoting CO₂ Electroreduction to Formate over a Wide Potential Window

Boron Dopant Induced Electron‐Rich Bismuth for Electrochemical CO₂ Reduction with High Solar Energy Conversion Efficiency