eprintid: 10197355 rev_number: 7 eprint_status: archive userid: 699 dir: disk0/10/19/73/55 datestamp: 2024-09-20 10:32:43 lastmod: 2024-09-20 10:32:43 status_changed: 2024-09-20 10:32:43 type: article metadata_visibility: show sword_depositor: 699 creators_name: Palanimuthu, Naveenkumar creators_name: Subramaniam, Mohan Raj creators_name: Austeria P, Muthu creators_name: Sharma, Preetam Kumar creators_name: Ramalingam, Vinoth creators_name: Peramaiah, Karthik creators_name: Ramakrishnan, Shanmugam creators_name: Gu, Geun Ho creators_name: Yu, Eileen Hao creators_name: Yoo, Dong Jin title: Surface Area-Enhanced Cerium and Sulfur-Modified Hierarchical Bismuth Oxide Nanosheets for Electrochemical Carbon Dioxide Reduction to Formate ispublished: inpress divisions: UCL divisions: B04 divisions: C06 divisions: F62 divisions: ZZN keywords: Bismuth oxide; density functional theory; electrochemical CO2 reduction; formate; surface area note: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. abstract: Electrochemical carbon dioxide reduction reaction (ECO2RR) is a promising approach to synthesize fuels and value-added chemical feedstocks while reducing atmospheric CO2 levels. Here, high surface area cerium and sulfur-doped hierarchical bismuth oxide nanosheets (Ce@S-Bi2O3) are develpoed by a solvothermal method. The resulting Ce@S-Bi2O3 electrocatalyst shows a maximum formate Faradaic efficiency (FE) of 92.5% and a current density of 42.09 mA cm−2 at −1.16 V versus RHE using a traditional H-cell system. Furthermore, using a three-chamber gas diffusion electrode (GDE) reactor, a maximum formate FE of 85% is achieved in a wide range of applied potentials (−0.86 to −1.36 V vs RHE) using Ce@S-Bi2O3. The density functional theory (DFT) results show that doping of Ce and S in Bi2O3 enhances formate production by weakening the OH* and H* species. Moreover, DFT calculations reveal that *OCHO is a dominant pathway on Ce@S-Bi2O3 that leads to efficient formate production. This study opens up new avenues for designing metal and element-doped electrocatalysts to improve the catalytic activity and selectivity for ECO2RR. date: 2024-06-07 date_type: published publisher: WILEY-V C H VERLAG GMBH official_url: http://dx.doi.org/10.1002/smll.202400913 full_text_type: other language: eng verified: verified_manual elements_id: 2284358 doi: 10.1002/smll.202400913 medium: Print-Electronic lyricists_name: Sharma, Preetam Kumar lyricists_id: PKSHA76 actors_name: Sharma, Preetam Kumar actors_id: PKSHA76 actors_role: owner funding_acknowledgements: [Jeonbuk National University Research]; 2023RIS-008 [BK21 FOUR Program by Jeonbuk National University Research Grant]; NRF-2020R1A2B5B01001458 [Regional Innovation Strategy (RIS)" through the National Research Foundation of Korea (NRF) - Ministry of Education (MOE)]; [Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Science, ICT and Future Planning]; EP/V011863/1 [Korea Institute of Science and Technology Information (KISTI)]; [UKRI Circular Chemical Economy Centre] full_text_status: restricted publication: Small article_number: 2400913 pages: 12 event_location: Germany issn: 1613-6810 citation: Palanimuthu, Naveenkumar; Subramaniam, Mohan Raj; Austeria P, Muthu; Sharma, Preetam Kumar; Ramalingam, Vinoth; Peramaiah, Karthik; Ramakrishnan, Shanmugam; ... Yoo, Dong Jin; + view all <#> Palanimuthu, Naveenkumar; Subramaniam, Mohan Raj; Austeria P, Muthu; Sharma, Preetam Kumar; Ramalingam, Vinoth; Peramaiah, Karthik; Ramakrishnan, Shanmugam; Gu, Geun Ho; Yu, Eileen Hao; Yoo, Dong Jin; - view fewer <#> (2024) Surface Area-Enhanced Cerium and Sulfur-Modified Hierarchical Bismuth Oxide Nanosheets for Electrochemical Carbon Dioxide Reduction to Formate. Small , Article 2400913. 10.1002/smll.202400913 <https://doi.org/10.1002/smll.202400913>. (In press). document_url: https://discovery.ucl.ac.uk/id/eprint/10197355/1/Small%202024%20accepted%20final%20manuscript.pdf