Structural reconstruction of carbon nitride with tailored electronic structure: A bifunctional photocatalyst for cooperative artificial photosynthesis and selective phenylcarbinol oxidation
Structural reconstruction of carbon nitride with tailored electronic structure: A bifunctional photocatalyst for cooperative artificial photosynthesis and selective phenylcarbinol oxidation
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DOI：
10.1016/j.apcatb.2021.120517
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发表时间：
2021-12
影响因子：
22.1
通讯作者：
Zailun Liu;Zejun Zhao;Wenjun Jiang;Zi-zhong Zhu;Yuhong Wang;Zhe Liu;Wenhao Gu;Yang Yang-Yang;
中科院分区：
文献类型：
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作者：
Zailun Liu;Zejun Zhao;Wenjun Jiang;Zi-zhong Zhu;Yuhong Wang;Zhe Liu;Wenhao Gu;Yang Yang-Yang;
在此，通过在氮气气氛中简单地煅烧硼氢化钠和CN纳米片（CNS）来重构和定制氮化碳的电子结构，这可以促进电荷载流子的面内分离和输运。因此，CNS的结构重构表现出突出的CO2减排性能（55.3 μmol g−1h−1）和高CO选择性（98.9%），不含任何助催化剂和牺牲剂，约为本体CN的10倍（5.7 μmol g−1h−1），由于降低了吸附 *COOH中间体的限速步骤的势垒能并降低了价带（VB）用于增加水氧化驱动力的位置。更重要的是，R-CNS-400可以选择性地将苯甲醇氧化为苯甲醛（选择性/99.3%），同时将CO2还原为CO。这项工作为设计具有增加的水氧化驱动力和增强的电荷分离的CN基材料提供了新的见解，以通过结构重构实现高效CO2光还原。
Herein, electronic structure of carbon nitride is reconstructed and tailored by simply calcining the sodium borohydride and CN nanosheets (CNS) in a nitrogen atmosphere, which could promote the in-plane separation and transport of charge carriers. Accordingly, structural reconstruction of CNS manifests outstanding CO2reduction performance (55.3 μmol g−1h−1) and high CO selectivity (98.9 %) without any cocatalysts and sacrificial agents, roughly 10-fold of bulk CN (5.7 μmol g−1h−1), owing to decrease the barrier energy of rate-limiting step for adsorbed *COOH intermediate and lower the valence band (VB) position for increasing the water oxidation driving force. More importantly, the R-CNS-400 can selectively oxidize the phenylcarbinol to phenyl methanal (selectivity/99.3 %) and simultaneously reduce CO2to CO. This work provides new insights for designing CN-based materials with increased water oxidation driving force and enhanced charge separation for high efficiency CO2photoreduction by structural reconstruction.