具有表面和界面双极化的空位对诱导电荷再平衡用于 CO2 光还原,ACS Catalysis

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具有表面和界面双极化的空位对诱导电荷再平衡用于 CO2 光还原
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-12-07 , DOI: 10.1021/acscatal.2c04675
Jun Di _{1,

2} , Xingwang Zhu ₃ , Gazi Hao ₁ , Chao Zhu ₂ , Hailong Chen ₄ , Qiaoxi Liu ₅ , Ruihuan Duan ₂ , Hongwei Hu ₂ , Yi Zhang ₆ , Jun Xiong ₆ , Ran Long ₅ , Jiexiang Xia ₆ , Yu-Xiang Weng ₄ , Wei Jiang ₁ , Zheng Liu ₂

Affiliation

不良的电荷动力学大大降低了光催化CO ₂还原的效率。在此，开发了同步表面和界面双极化策略以促进电荷分离。Bi ₂₄ O ₃₁ Br ₁₀原子层中的 Bi-O 空位对可以触发黑磷 (BP) 和 Bi ₂₄ O ₃₁ Br ₁₀之间的强耦合，形成结构紧密接触的 BP-Bi ₂₄ O ₃₁ Br ₁₀配置，电荷-通过电负性引起的电荷再平衡重新分布界面。_{Bi 24} O ₃₁ Br表面的 Bi-O 空位对₁₀和重组的 BP/Bi ₂₄ O ₃₁ Br ₁₀界面实现同步表面和界面双极化，创建从 Bi ₂₄ O ₃₁ Br ₁₀内部到 BP 表面的电子桥，如超快瞬态吸收光谱所证明的那样。这种配置有利于降低 CO ₂活化能垒，有效稳定 COOH* 中间体，并降低决速步骤能垒。受益于这些特性，优化后的 BP–Bi ₂₄ O ₃₁ Br ₁₀的稳定 CO 生成率高达 39.8 μmol g ^–1 h ^–1通过水中的CO _{2光还原，分别是有缺陷的Bi}₂₄ O ₃₁ Br ₁₀原子层和缺乏缺陷的Bi ₂₄ O ₃₁ Br ₁₀的2.4和46.8倍。本研究为双极化的表面缺陷和重组界面的同步设计提供了见解。

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Vacancy Pair-Induced Charge Rebalancing with Surface and Interfacial Dual Polarization for CO2 Photoreduction

Poor charge kinetics greatly reduce the efficiency of photocatalytic CO₂ reduction. Herein, a synchronous surface and interfacial dual polarization strategy was developed to promote charge separation. Bi–O vacancy pairs in Bi₂₄O₃₁Br₁₀ atomic layers can trigger strong coupling between black phosphorus (BP) and Bi₂₄O₃₁Br₁₀, forming a restructured closely contacted BP–Bi₂₄O₃₁Br₁₀ configuration with a charge-redistributed interface via electronegativity-induced charge rebalancing. The Bi–O vacancy pairs on the surface of Bi₂₄O₃₁Br₁₀ and restructured BP/Bi₂₄O₃₁Br₁₀ interface enable synchronous surface and interfacial dual polarization, creating an electronic bridge from the interior of Bi₂₄O₃₁Br₁₀ to the BP surface, as proven by ultrafast transient absorption spectroscopy. This configuration favors a low CO₂ activation energy barrier, effectively stabilizes COOH* intermediates, and decreases the rate-determining step energy barrier. Benefiting from these features, the stable CO generation rate of optimized BP–Bi₂₄O₃₁Br₁₀ reaches up to 39.8 μmol g^–1 h^–1 via CO₂ photoreduction in water, which is 2.4 and 46.8 times higher than those of defective Bi₂₄O₃₁Br₁₀ atomic layers and defect-poor Bi₂₄O₃₁Br₁₀, respectively. This study provides insights into the synchronous design of surface defects and restructured interfaces for dual polarization.

更新日期：2022-12-07

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