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用于增强光催化析氢并耦合苯甲醇选择性氧化的新型有机-无机Z型异质结

Novel organic-inorganic Z-scheme heterojunction for enhanced photocatalytic hydrogen evolution coupled with selective oxidation of benzyl alcohol oxidation.

作者信息

You Chuanxu, Guo Pengyu, Zhang Baining, Zhang Peng, Wang Runwei, Zhang Zongtao, Qiu Shilun

机构信息

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

出版信息

J Colloid Interface Sci. 2025 Dec 15;700(Pt 3):138563. doi: 10.1016/j.jcis.2025.138563. Epub 2025 Jul 27.

Abstract

The development of a synergistic dual-functional photocatalyst for hydrogen (H) evolution and the value-added oxidation of benzyl alcohol (BA) is of great significance for both energy conversion and organic synthesis. In this study, a porous Z-scheme heterojunction photocatalyst (MnCd)(CNS)/MnCdS (MCTMT/MCS) was successfully constructed via a simple wet-chemical method combined with hydrothermal decomposition. By controlling the hydrothermal decomposition process, the specific surface area of the catalyst was significantly increased from 15.71 m/g to 202.77 m/g, which is conducive to the enhanced contact between reactant molecules and the surface of the photocatalyst, thereby increasing the probability of the photocatalytic reaction. Under visible light irradiation, the optimal MCTMT/MCS heterojunction exhibited outstanding photocatalytic performance, with an H₂ evolution rate of 1.42 mmol·g·h and a BA conversion rate exceeding 90 %, which is seventeen times higher than MCTMT. After 25 h of cyclic testing, the H₂ evolution rate remained at 1.12 mmol·g·h, significantly surpassing that of single-component catalysts. Moreover, UPS analysis elucidated the specific electron transfer pathway in the Z-scheme heterostructure of MCTMT/MCS, revealing that efficient charge separation and transfer significantly enhanced photocatalytic activity. This study provides valuable insights into the design of synergistic bifunctional metal sulfide photocatalysts for photocatalytic green H production and the synthesis of high value chemicals.

摘要

开发一种用于析氢和苯甲醇(BA)增值氧化的协同双功能光催化剂,对于能量转换和有机合成均具有重要意义。在本研究中,通过简单的湿化学方法结合水热分解成功构建了一种多孔Z型异质结光催化剂(MnCd)(CNS)/MnCdS(MCTMT/MCS)。通过控制水热分解过程,催化剂的比表面积从15.71 m²/g显著增加到202.77 m²/g,这有利于反应物分子与光催化剂表面之间增强接触,从而增加光催化反应的概率。在可见光照射下,最佳的MCTMT/MCS异质结表现出优异的光催化性能,析氢速率为1.42 mmol·g⁻¹·h⁻¹,BA转化率超过90%,比MCTMT高17倍。经过25小时的循环测试后,析氢速率保持在1.12 mmol·g⁻¹·h⁻¹,显著超过单组分催化剂。此外,UPS分析阐明了MCTMT/MCS的Z型异质结构中的特定电子转移途径,表明有效的电荷分离和转移显著增强了光催化活性。本研究为用于光催化绿色制氢和高价值化学品合成的协同双功能金属硫化物光催化剂的设计提供了有价值的见解。

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