碳点介导 Bi 簇在 g-C3N4 纳米网格上的原位限制生长以促进等离子体辅助 CO2 光还原,Small

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碳点介导 Bi 簇在 g-C3N4 纳米网格上的原位限制生长以促进等离子体辅助 CO2 光还原
Small ( IF 13.0 ) Pub Date : 2022-10-10 , DOI: 10.1002/smll.202204154
Xinyang Zhao ₁ , Jun Li ₂ , Xiangguang Kong ₁ , Changchang Li ₁ , Bo Lin ₃ , Fan Dong ₄ , Guidong Yang ₃ , Guosheng Shao ₁ , Chao Xue ₁

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鉴于其在新发展理念下实现碳中和目标的重要性，长期以来，合成高效、经济且稳定的光催化剂一直是可持续光催化 CO _{2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品选择性差仍然是 CRR 进展中的挑战。在此，这项工作揭示了高密度单分散 Bi/碳点 (CD) 和超薄石墨相氮化碳 (gC ₃ N ₄ ) 纳米网之间的协同效应，用于等离子体辅助光催化 CRR。最优 gC ₃ N ₄/Bi/CDs 异质结显示出 98% 的 CO 生产选择性，在没有任何牺牲剂的情况下产率高达 22.7 µmol g ^{−1 。}等离子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gC ₃ N ₄的电导率。同时，内置的电场驱动力调制等离子体Bi团簇和gC ₃ N ₄光敏单元定向注入光生空穴到相邻的CDs储层，从而促进CRR过程中的快速分离和定向转移。这项工作阐明了等离子体辅助光催化 CRR 的机理，并为设计高效的等离子体参与光催化剂提供了途径。

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Carbon Dots Mediated In Situ Confined Growth of Bi Clusters on g-C3N4 Nanomeshes for Boosting Plasma-Assisted Photoreduction of CO2

Synthesis of high-efficiency, cost-effective, and stable photocatalysts has long been a priority for sustainable photocatalytic CO₂ 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-C₃N₄) nanomeshes for plasma-assisted photocatalytic CRR. The optimal g-C₃N₄/Bi/CDs heterojunction displays a high selectivity of 98% for CO production with a yield up to 22.7 µmol g⁻¹ 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-C₃N₄. Meanwhile, a built-in electric field driving force modulates the directional injection photogenerated holes from plasmonic Bi clusters and g-C₃N₄ 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.

更新日期：2022-10-10

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