High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress
Electroreduction of CO2 into formic acid (HCOOH) is of great economical value and potential for industrialization. However, it is still a substantial challenge due to the lack of efficient catalysts with simultaneously high activity, selectivity, and durability. Herein, a single‐atom bismuth loaded...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2024-01-01
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| Series: | Small Structures |
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| Online Access: | https://doi.org/10.1002/sstr.202300323 |
| _version_ | 1797361243772682240 |
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| author | Jihan Zhang Kun Zhao Yueming Ma Weirui Chen Xinglei Shi Chenghua Sun Qianyu Zhang Junfeng Niu |
| author_facet | Jihan Zhang Kun Zhao Yueming Ma Weirui Chen Xinglei Shi Chenghua Sun Qianyu Zhang Junfeng Niu |
| author_sort | Jihan Zhang |
| collection | DOAJ |
| description | Electroreduction of CO2 into formic acid (HCOOH) is of great economical value and potential for industrialization. However, it is still a substantial challenge due to the lack of efficient catalysts with simultaneously high activity, selectivity, and durability. Herein, a single‐atom bismuth loaded on N‐doped hollow carbon sphere (Bi–SA/NHCS) catalyst is reported and its catalytic activity and selectivity are modulated by changing the coordination structure of Bi center. The obtained Bi–SA/NHCS with a Bi–N3 site exhibits significantly enhanced electrocatalytic activity and selectivity of HCOOH synthesis from CO2 reduction. The HCOOH production rate achieves 16.2 mmol L−1 h−1 cm−2 at a current density of 20 mA cm−2, and its Faradaic efficiency remains 100% during a long‐term reaction. The HCOOH production rate normalized by catalyst loading is at a molar level of nearly 1.5 mol h−1 gcat−1. The production rate and Faradaic efficiency of HCOOH electrosynthesis on Bi–SA/NHCS are significantly boosted as compared with other catalysts reported in the literature. Experimental and density‐functional theory results demonstrate that the boosted activity and selectivity of HCOOH synthesis owe to the electronic structure modulation to the Bi center via threefold coordinated N‐ligands, leading to a proper binding energy of HOCO* intermediates. |
| first_indexed | 2024-03-08T15:51:07Z |
| format | Article |
| id | doaj.art-c867a4d72c30427090a03a8f48b1d077 |
| institution | Directory Open Access Journal |
| issn | 2688-4062 |
| language | English |
| last_indexed | 2024-03-08T15:51:07Z |
| publishDate | 2024-01-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Small Structures |
| spelling | doaj.art-c867a4d72c30427090a03a8f48b1d0772024-01-09T05:33:22ZengWiley-VCHSmall Structures2688-40622024-01-0151n/an/a10.1002/sstr.202300323High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon NanospheressJihan Zhang0Kun Zhao1Yueming Ma2Weirui Chen3Xinglei Shi4Chenghua Sun5Qianyu Zhang6Junfeng Niu7College of Environmental Science and Engineering North China Electric Power University Beinong Road 2 Beijing 102206 ChinaCollege of Environmental Science and Engineering North China Electric Power University Beinong Road 2 Beijing 102206 ChinaSchool of New Energy North China Electric Power University Beinong Road 2 Beijing 102206 ChinaSchool of Environmental Science and Engineering Guangdong University of Technology Huanxi Road 100 Guangzhou 510006 ChinaCollege of Environmental Science and Engineering North China Electric Power University Beinong Road 2 Beijing 102206 ChinaSchool of Chemistry and Biology Swinburne University of Technology John Street VIC 3122 AustraliaCollege of Materials Science and Engineering Sichuan University Chengdu 610065 ChinaCollege of Environmental Science and Engineering North China Electric Power University Beinong Road 2 Beijing 102206 ChinaElectroreduction of CO2 into formic acid (HCOOH) is of great economical value and potential for industrialization. However, it is still a substantial challenge due to the lack of efficient catalysts with simultaneously high activity, selectivity, and durability. Herein, a single‐atom bismuth loaded on N‐doped hollow carbon sphere (Bi–SA/NHCS) catalyst is reported and its catalytic activity and selectivity are modulated by changing the coordination structure of Bi center. The obtained Bi–SA/NHCS with a Bi–N3 site exhibits significantly enhanced electrocatalytic activity and selectivity of HCOOH synthesis from CO2 reduction. The HCOOH production rate achieves 16.2 mmol L−1 h−1 cm−2 at a current density of 20 mA cm−2, and its Faradaic efficiency remains 100% during a long‐term reaction. The HCOOH production rate normalized by catalyst loading is at a molar level of nearly 1.5 mol h−1 gcat−1. The production rate and Faradaic efficiency of HCOOH electrosynthesis on Bi–SA/NHCS are significantly boosted as compared with other catalysts reported in the literature. Experimental and density‐functional theory results demonstrate that the boosted activity and selectivity of HCOOH synthesis owe to the electronic structure modulation to the Bi center via threefold coordinated N‐ligands, leading to a proper binding energy of HOCO* intermediates.https://doi.org/10.1002/sstr.202300323CO2 reductionscoordination structuresHCOOH productionssingle-atom bismuth |
| spellingShingle | Jihan Zhang Kun Zhao Yueming Ma Weirui Chen Xinglei Shi Chenghua Sun Qianyu Zhang Junfeng Niu High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress Small Structures CO2 reductions coordination structures HCOOH productions single-atom bismuth |
| title | High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress |
| title_full | High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress |
| title_fullStr | High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress |
| title_full_unstemmed | High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress |
| title_short | High‐Yield Electrosynthesis of Formic Acid from CO2 Reduction on Single‐Bismuth Catalyst Loaded on N‐Doped Hollow Carbon Nanospheress |
| title_sort | high yield electrosynthesis of formic acid from co2 reduction on single bismuth catalyst loaded on n doped hollow carbon nanospheress |
| topic | CO2 reductions coordination structures HCOOH productions single-atom bismuth |
| url | https://doi.org/10.1002/sstr.202300323 |
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