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Article: Tuning Metal-Free Hierarchical Boron Nitride-like Catalyst for Enhanced Photocatalytic CO2Reduction Activity

TitleTuning Metal-Free Hierarchical Boron Nitride-like Catalyst for Enhanced Photocatalytic CO<inf>2</inf>Reduction Activity
Authors
Keywordsboron nitride-like catalyst
hierarchical architecture
metal-free
photocatalytic CO reduction 2
reaction mechanism
Issue Date2022
Citation
ACS Catalysis, 2022, v. 12, n. 19, p. 12217-12226 How to Cite?
AbstractBoron nitride (BN)-based materials, which are commonly used as metal-free catalysts for thermal catalysis and pollution degradation, have shown potential for photocatalytic reduction of CO2into valuable carbon fuels. However, the poor performance and the insufficient explanation of the reaction mechanism of the very few reported BN-based catalysts still seriously restrict the practical development. Herein, we synthesize a hierarchical BN-like flower catalyst composed of nanofibers (∼50 nm) by combining an in situ self-assembly strategy with a self-modification method. The photocatalytic CO2-to-CO reduction rate of BN-like flowers with low B-O species content is over 3-fold than that of BN-like flowers with high B-O species content and even more than 26.7 and 7.3 times than that of bulk BN and bulk carbon nitride (CN), respectively. Notably, the performance of the as-prepared catalysts is much higher than that of the reported BN-based catalysts and nearly all the popular metal-free CN and even comparable to most metal-based catalysts. Importantly, we in-depth investigate the reasons and mechanisms for the enhancement of photocatalytic CO2reduction activity of BN-like flowers by combining various advanced characterizations and DFT calculations. It is found that in the BN-like flowers, B atoms linked to O atoms act as active sites, and the low B-O species content is beneficial for dynamic charge transfer and *CO desorption. In addition, the catalyst also shows good stability which is verified by cycling experiments together with molecular dynamics computation. The synthesis of the metal-free BN-based catalyst and systematic theoretical investigation will be beneficial to the development of advanced catalysts for solar fuel production.
Persistent Identifierhttp://hdl.handle.net/10722/326364
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorLiang, Jianli-
dc.contributor.authorZhang, Wei-
dc.contributor.authorLiu, Zheyang-
dc.contributor.authorSong, Qianqian-
dc.contributor.authorZhu, Zhaohua-
dc.contributor.authorGuan, Zhiqiang-
dc.contributor.authorWang, Heyi-
dc.contributor.authorZhang, Pengjun-
dc.contributor.authorLi, Jing-
dc.contributor.authorZhou, Min-
dc.contributor.authorCao, Chen-
dc.contributor.authorXu, Hui-
dc.contributor.authorLu, Yang-
dc.contributor.authorMeng, Xiangmin-
dc.contributor.authorSong, Li-
dc.contributor.authorWong, Po Keung-
dc.contributor.authorJiang, Zhifeng-
dc.contributor.authorLee, Chun Sing-
dc.date.accessioned2023-03-09T10:00:05Z-
dc.date.available2023-03-09T10:00:05Z-
dc.date.issued2022-
dc.identifier.citationACS Catalysis, 2022, v. 12, n. 19, p. 12217-12226-
dc.identifier.urihttp://hdl.handle.net/10722/326364-
dc.description.abstractBoron nitride (BN)-based materials, which are commonly used as metal-free catalysts for thermal catalysis and pollution degradation, have shown potential for photocatalytic reduction of CO2into valuable carbon fuels. However, the poor performance and the insufficient explanation of the reaction mechanism of the very few reported BN-based catalysts still seriously restrict the practical development. Herein, we synthesize a hierarchical BN-like flower catalyst composed of nanofibers (∼50 nm) by combining an in situ self-assembly strategy with a self-modification method. The photocatalytic CO2-to-CO reduction rate of BN-like flowers with low B-O species content is over 3-fold than that of BN-like flowers with high B-O species content and even more than 26.7 and 7.3 times than that of bulk BN and bulk carbon nitride (CN), respectively. Notably, the performance of the as-prepared catalysts is much higher than that of the reported BN-based catalysts and nearly all the popular metal-free CN and even comparable to most metal-based catalysts. Importantly, we in-depth investigate the reasons and mechanisms for the enhancement of photocatalytic CO2reduction activity of BN-like flowers by combining various advanced characterizations and DFT calculations. It is found that in the BN-like flowers, B atoms linked to O atoms act as active sites, and the low B-O species content is beneficial for dynamic charge transfer and *CO desorption. In addition, the catalyst also shows good stability which is verified by cycling experiments together with molecular dynamics computation. The synthesis of the metal-free BN-based catalyst and systematic theoretical investigation will be beneficial to the development of advanced catalysts for solar fuel production.-
dc.languageeng-
dc.relation.ispartofACS Catalysis-
dc.subjectboron nitride-like catalyst-
dc.subjecthierarchical architecture-
dc.subjectmetal-free-
dc.subjectphotocatalytic CO reduction 2-
dc.subjectreaction mechanism-
dc.titleTuning Metal-Free Hierarchical Boron Nitride-like Catalyst for Enhanced Photocatalytic CO<inf>2</inf>Reduction Activity-
dc.typeArticle-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1021/acscatal.2c03970-
dc.identifier.scopuseid_2-s2.0-85139199411-
dc.identifier.volume12-
dc.identifier.issue19-
dc.identifier.spage12217-
dc.identifier.epage12226-
dc.identifier.eissn2155-5435-
dc.identifier.isiWOS:000862366800001-

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