Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals
Converting CO2 and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy issues. Taking inspiration from the structures of natural leaves, we designed and synthesized a novel copper-coordinated covalent triazine framework (CuCTF) supp...
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| Format: | Article |
| Language: | English |
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KeAi Communications Co., Ltd.
2025-02-01
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| Series: | Green Energy & Environment |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2468025724001067 |
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| author | Wenrui Wan Fanhua Meng Si Chen Jianhua Wang Chunyan Liu Yan Wei Chenpu He Li Fan Qiaolan Zhang Weichun Ye Huanwang Jing |
| author_facet | Wenrui Wan Fanhua Meng Si Chen Jianhua Wang Chunyan Liu Yan Wei Chenpu He Li Fan Qiaolan Zhang Weichun Ye Huanwang Jing |
| author_sort | Wenrui Wan |
| collection | DOAJ |
| description | Converting CO2 and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy issues. Taking inspiration from the structures of natural leaves, we designed and synthesized a novel copper-coordinated covalent triazine framework (CuCTF) supported by silicon nanowire arrays on wafer chip. This marks the first-ever application of such a hybrid material in the photoelectrocatalytic reduction of CO2 under mild conditions. The Si@CuCTF6 heterojunction has exhibited exceptional selectivity of 95.6% towards multicarbon products (C2+) and apparent quantum efficiency (AQE) of 0.89% for carbon-based products. The active sites of the catalysts are derived from the nitrogen atoms of unique triazine ring structure in the ordered porous framework and the abundant Cu–N coordination sites with bipyridine units. Furthermore, through DFT calculations and operando FTIR spectra analysis, we proposed a comprehensive mechanism for the photoelectrocatalytic CO2 reduction, confirming the existence of key intermediate species such as ∗CO2−, ∗=C=O, ∗CHO and ∗CO–CHO etc. This work not only provides a new way to mimic photosynthesis of plant leaves but also gives a new opportunity to enter this research field in the future. |
| format | Article |
| id | doaj-art-4df294c387a4432c8d16bef348bb4aa7 |
| institution | DOAJ |
| issn | 2468-0257 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | KeAi Communications Co., Ltd. |
| record_format | Article |
| series | Green Energy & Environment |
| spelling | doaj-art-4df294c387a4432c8d16bef348bb4aa72025-08-20T02:43:43ZengKeAi Communications Co., Ltd.Green Energy & Environment2468-02572025-02-0110242243210.1016/j.gee.2024.04.007Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicalsWenrui Wan0Fanhua Meng1Si Chen2Jianhua Wang3Chunyan Liu4Yan Wei5Chenpu He6Li Fan7Qiaolan Zhang8Weichun Ye9Huanwang Jing10State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, China; Key Laboratory of Green Chemical Media and Reactions (Ministry of Education), School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, 453007, Henan, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, ChinaSchool of Chemical Engineering, Lanzhou University of Arts and Sciences, Lanzhou, 730010, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, ChinaState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, China; Corresponding authors.State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, China; Corresponding authors.State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, Gansu, China; Corresponding authors.Converting CO2 and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy issues. Taking inspiration from the structures of natural leaves, we designed and synthesized a novel copper-coordinated covalent triazine framework (CuCTF) supported by silicon nanowire arrays on wafer chip. This marks the first-ever application of such a hybrid material in the photoelectrocatalytic reduction of CO2 under mild conditions. The Si@CuCTF6 heterojunction has exhibited exceptional selectivity of 95.6% towards multicarbon products (C2+) and apparent quantum efficiency (AQE) of 0.89% for carbon-based products. The active sites of the catalysts are derived from the nitrogen atoms of unique triazine ring structure in the ordered porous framework and the abundant Cu–N coordination sites with bipyridine units. Furthermore, through DFT calculations and operando FTIR spectra analysis, we proposed a comprehensive mechanism for the photoelectrocatalytic CO2 reduction, confirming the existence of key intermediate species such as ∗CO2−, ∗=C=O, ∗CHO and ∗CO–CHO etc. This work not only provides a new way to mimic photosynthesis of plant leaves but also gives a new opportunity to enter this research field in the future.http://www.sciencedirect.com/science/article/pii/S2468025724001067SiliconPhotoelectrocatalysisCO2 reductionCovalent triazine frameworkSustainable chemistry |
| spellingShingle | Wenrui Wan Fanhua Meng Si Chen Jianhua Wang Chunyan Liu Yan Wei Chenpu He Li Fan Qiaolan Zhang Weichun Ye Huanwang Jing Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals Green Energy & Environment Silicon Photoelectrocatalysis CO2 reduction Covalent triazine framework Sustainable chemistry |
| title | Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals |
| title_full | Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals |
| title_fullStr | Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals |
| title_full_unstemmed | Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals |
| title_short | Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals |
| title_sort | triazine cof silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic co2 reduction to c2 chemicals |
| topic | Silicon Photoelectrocatalysis CO2 reduction Covalent triazine framework Sustainable chemistry |
| url | http://www.sciencedirect.com/science/article/pii/S2468025724001067 |
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