分子筛介导的氧化铟催化剂用于增强光催化CO2加氢

doi:10.1016/j.actphy.2025.100133

物理化学学报 >> 2025, Vol. 41 >> Issue (11): 100133.doi: 10.1016/j.actphy.2025.100133

分子筛介导的氧化铟催化剂用于增强光催化CO₂加氢

管勤辉¹, 郭昱昊¹, 李娜²^,*(), 李敬³, 颜廷江¹^,²^,*()

¹ 陕西科技大学化学与化工学院, 陕西西安 710021
² 曲阜师范大学化学与化工学院, 山东曲阜 273165
³ 中国科学院理化技术研究所光化学转换与光电材料重点实验室, 北京 100190

收稿日期:2025-06-16 修回日期:2025-07-18 录用日期:2025-07-20 发布日期:2025-09-29
通讯作者: Email: lina20201130@163.com (李娜)tingjiangn@163.com (颜廷江)
基金资助:
国家自然科学基金(22172086); 国家自然科学基金(22105117); 山东省泰山学者计划(tsqn202103064); 山东省重大基础研究项目(ZR2021ZD06)

Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO₂ hydrogenation

Qinhui Guan¹, Yuhao Guo¹, Na Li²^,*(), Jing Li³, Tingjiang Yan¹^,²^,*()

¹ College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi'an 710021, Shannxi Province, China
² School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu 273165, Shandong Province, China
³ Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Received:2025-06-16 Revised:2025-07-18 Accepted:2025-07-20 Published:2025-09-29
Contact: Email: lina20201130@163.com (Na Li)tingjiangn@163.com (Tingjiang Yan)
Supported by:
the National Natural Science Foundation of China(22172086); the National Natural Science Foundation of China(22105117); the Taishan Scholars Program of Shandong Province(tsqn202103064); the Major Basic Research Project of Shandong Province(ZR2021ZD06)

1. ACTPHY-2025.100133-SI-12p.pdf(10200KB)

摘要/Abstract

摘要：

在光催化CO₂加氢领域，光生载流子的吸附-脱附行为及其动力学特性是影响光催化反应动力学过程与整体效率的关键因素。本文通过简便的浸渍-煅烧法制备了5A分子筛功能化的In₂O₃复合材料(记为IO@5A-xwt%)。其中，经5A分子筛负载量优化的IO@5A-5wt%复合材料在光催化CO₂转化为CO的反应中表现出色，CO生成速率达到2610.55 μmol·g⁻¹·h⁻¹，为原始In₂O₃的19倍。此外，IO@5A-5wt%复合材料在经过持续45 h、总计108次循环的长时间测试后仍保持可接受的催化稳定性。一系列全面的表征技术和性能评估表明，5A分子筛的引入显著调节了光催化反应中的吸附-脱附行为和空穴动力学。5A分子筛的多通道结构具有合适的孔径，有效增强了CO₂的吸附。同时，5A分子筛的表面羟基促进了光生空穴的转移，从而抑制了光生载流子的复合。此外，反应产物H₂O更容易从催化剂表面脱附。这些协同效应共同构成了IO@5A-5wt%复合材料光催化性能增强的关键机制。

关键词: 分子筛, In₂O₃, 分子选择性储层, 光催化, CO₂加氢

Abstract:

In the realm of photocatalytic CO₂ hydrogenation, the adsorption-desorption behaviors and dynamics of photogenerated carriers are pivotal determinants of the kinetic processes and overall efficiency of photocatalytic reactions. Herein, 5A molecular sieve-functionalized In₂O₃ composites (denoted as IO@5A-xwt%) were fabricated through a facile impregnation-calcination method. Among them, the IO@5A-5wt% composite, with the optimized loading amount of 5A molecular sieves, showcases outstanding performance in photocatalytic conversion of CO₂ to CO, achieving a CO production rate of 2610.55 μmol·g⁻¹·h⁻¹, which is 19 times higher than that of pristine In₂O₃. Moreover, the IO@5A-5wt% composite maintains acceptable catalytic stability after a prolonged experiment lasting 45 h and total of 108 cycles. A comprehensive series of characterization techniques and performance evaluations reveal that the incorporation of 5A molecular sieves significantly modulates the adsorption-desorption behavior and hole dynamics during photocatalytic reactions. The multi-channel architecture of 5A molecular sieves, featuring suitable pore sizes, effectively enhances CO₂ adsorption. Meanwhile, the surface hydroxyl groups of 5A molecular sieves facilitate the transfer of photogenerated holes, thereby suppressing the recombination of photogenerated carriers. Additionally, the reaction product H₂O desorbs more readily from the catalyst surface. These synergistic effects collectively constitute the key mechanism underlying the enhanced photocatalytic performance of the IO@5A-5wt% composite.

Key words: Molecular sieve, In₂O₃, Molecular-selective reservoir, Photocatalysis, CO₂ hydrogenation

管勤辉, 郭昱昊, 李娜, 李敬, 颜廷江. 分子筛介导的氧化铟催化剂用于增强光催化CO₂加氢[J]. 物理化学学报, 2025, 41(11), 100133. doi: 10.1016/j.actphy.2025.100133

Qinhui Guan, Yuhao Guo, Na Li, Jing Li, Tingjiang Yan. Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO₂ hydrogenation[J]. Acta Phys. -Chim. Sin. 2025, 41(11), 100133. doi: 10.1016/j.actphy.2025.100133

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100133

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I11/100133

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分子筛介导的氧化铟催化剂用于增强光催化CO₂加氢

Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO₂ hydrogenation

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