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碳点介导Bi团簇在g-C₃N纳米网原位受限生长以促进等离子体辅助CO光还原

Carbon Dots Mediated In Situ Confined Growth of Bi Clusters on g-C N Nanomeshes for Boosting Plasma-Assisted Photoreduction of CO.

作者信息

Zhao Xinyang, Li Jun, Kong Xiangguang, Li Changchang, Lin Bo, Dong Fan, Yang Guidong, Shao Guosheng, Xue Chao

机构信息

State Centre for International Cooperation on Designer Low-carbon and Environmental Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, China.

Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou, 450052, China.

出版信息

Small. 2022 Nov;18(46):e2204154. doi: 10.1002/smll.202204154. Epub 2022 Oct 10.

Abstract

Synthesis of high-efficiency, cost-effective, and stable photocatalysts has long been a priority for sustainable photocatalytic CO reduction reactions (CRR), given its importance in achieving carbon neutrality goals under the new development philosophy. Fundamentally, the sluggish interface charge transportation and poor selectivity of products remain a challenge in the CRR progress. Herein, this work unveils a synergistic effect between high-density monodispersed Bi/carbon dots (CDs) and ultrathin graphite phase carbon nitride (g-C N ) nanomeshes for plasma-assisted photocatalytic CRR. The optimal g-C N /Bi/CDs heterojunction displays a high selectivity of 98% for CO production with a yield up to 22.7 µmol g without any sacrificial agent. The in situ confined growth of plasmonic Bi clusters favors the production of more hot carriers and improves the conductivity of g-C N . Meanwhile, a built-in electric field driving force modulates the directional injection photogenerated holes from plasmonic Bi clusters and g-C N photosensitive units to adjacent CDs reservoirs, thus promoting the rapid separation and oriented transfer in the CRR process. This work sheds light on the mechanism of plasma-assisted photocatalytic CRR and provides a pathway for designing highly efficient plasma-involved photocatalysts.

摘要

鉴于高效、经济高效且稳定的光催化剂的合成在新发展理念下实现碳中和目标方面的重要性,长期以来一直是可持续光催化CO还原反应(CRR)的优先事项。从根本上说,界面电荷传输缓慢和产物选择性差仍然是CRR进展中的一个挑战。在此,这项工作揭示了高密度单分散Bi/碳点(CDs)与超薄石墨相氮化碳(g-CN)纳米网在等离子体辅助光催化CRR中的协同效应。最佳的g-CN/Bi/CDs异质结在不使用任何牺牲剂的情况下,对CO生成显示出98%的高选择性,产率高达22.7 µmol g。等离子体Bi团簇的原位受限生长有利于产生更多的热载流子,并提高g-CN的导电性。同时,内置电场驱动力调节光生空穴从等离子体Bi团簇和g-CN光敏单元向相邻CDs储库的定向注入,从而促进CRR过程中的快速分离和定向转移。这项工作揭示了等离子体辅助光催化CRR的机制,并为设计高效的等离子体参与光催化剂提供了一条途径。

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