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在ZnIn₂S₄上进行D频段状态控制工程,以增强CO₂到CH₄的光降解

Benkun Wang¹, Guochao Shan², Yuheng Zhang¹

¹MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001 China.

Journal of colloid and interface science

|February 2, 2025

概括

在d10金属光催化剂中调节d波段中心可增强CO2到CH4的转化. 用ZnIn₂S₄与Bi等电子阴性元素进行兴奋剂,显著提高了甲选择性和光催化CO₂减少的产量.

科学领域:

材料科学材料科学材料科学
催化剂是一种催化剂.
摄影化学的使用.

背景情况:

具有d¹⁰电子配置的金属基光催化剂显示出减少CO2的希望.
在d¹⁰金属位点和CO₂之间的弱结合限制了CH₄生产的活性和选择性.
优化d波段中心对于增强光催化CO₂到CH₄转换至关重要.

研究的目的:

提出并验证一种策略,用于调节d金属光催化剂的d频段中心.
在光催化CO2降解过程中增强CH4的选择性和产量.
为了研究兴奋剂电子负元素对ZnIn₂S₄ (ZIS) 的作用,以改善CO₂光降解.

主要方法:

使用高度负电子元素 (Bi,Cu,Co) 合成化ZnIn₂S₄ (ZIS) 光催化剂.
可见光驱动的CO2减少实验,以评估光催化性能.
密度函数理论 (DFT) 计算以了解电子结构和反应机制.

主要成果:

用电子阴性元素杂ZIS使CO2光降解产品从CO转移到CO和CH4的混合物,其中CH4是主要产品.
双化ZIS (Bi-ZIS) 表现出最高的性能,达到63.68%的CH4选择性和21.07μmol·g-1·h-1的演化率.
DFT计算证实,兴奋剂上调了d频段中心,降低了CO2转化为CH4的能量屏障,并增强了中间结合.

结论:

该d频段中心调制策略有效地增强了CH4形成在光催化CO2减少使用d10金属光催化剂.
双化ZIS显示出CH₄生产的优越活性和选择性,验证了拟议的战略.
这项工作为优化10种基于金属的光催化剂提供了一种新的方法,以实现高效的CO2减少和转化.

关键词:

CH(4) 形成的形成.阳离子交换所阳离子交换所 D(10) 的电子配置.在D频段中部的D频段中.光催化CO2的降解演变.

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