通过边缘活性位点调控解析光热催化中析氢与二氧化碳还原的界面竞争

doi:10.1016/j.actphy.2025.100099

物理化学学报 >> 2025, Vol. 41 >> Issue (9): 100099.doi: 10.1016/j.actphy.2025.100099

通过边缘活性位点调控解析光热催化中析氢与二氧化碳还原的界面竞争

洪佳楠, 许辰宇*(), 刘烟, 黎昌棋, 王梦琳, 张彦威*()

浙江大学清洁能源利用国家重点实验室, 浙江杭州 310027

收稿日期:2025-03-22 修回日期:2025-04-19 录用日期:2025-04-28 发布日期:2025-07-04
通讯作者: Email: mrxcy@zju.edu.cn (许辰宇)zhangyw@zju.edu.cn (张彦威)
基金资助:
浙江省自然科学基金(LDT23E06014E06); 国家自然科学基金(52341602); 浙江省自然科学基金(LQ24E060001); 国家重点研发计划(2023YFC3710800); 中央高校基本科研业务费专项资金(2022ZFJH04)

Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis

Jianan Hong, Chenyu Xu*(), Yan Liu, Changqi Li, Menglin Wang, Yanwei Zhang*()

State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang Province, China

Received:2025-03-22 Revised:2025-04-19 Accepted:2025-04-28 Published:2025-07-04
Contact: Email: mrxcy@zju.edu.cn (Chenyu Xu)zhangyw@zju.edu.cn (Yanwei Zhang)
Supported by:
the Zhejiang Provincial Natural Science Foundation of China(LDT23E06014E06); the National Natural Science Foundation of China(52341602); the Zhejiang Provincial Natural Science Foundation of China(LQ24E060001); the National Key Research and Development Project(2023YFC3710800); the Fundamental Research Funds for the Central Universities(2022ZFJH04)

1. ACTPHY-2025.100099-SI-13p.pdf(13190KB)

摘要/Abstract

摘要：

太阳能驱动的光热催化CO₂与H₂O转化是生产可持续燃料和化学品的重要途径。然而，析氢反应(HER)与CO₂还原反应(CO₂RR)之间的竞争导致产物选择性不理想。贵金属纳米颗粒作为常用助催化剂，可在半导体上形成活性位点，其中金属-半导体界面边缘的特殊活性位点在竞争机制中起关键作用。本研究制备了具有丰富界面边缘位点的Al掺杂SrTiO₃负载贵金属催化剂，用于连续光热催化CO₂和H₂O转化。不同贵金属纳米颗粒上CO₂对析氢性能的影响表现出显著差异。通过原位漫反射红外傅里叶变换光谱(DRIFTS)和密度泛函理论(DFT)计算研究了关键中间基团的相互作用，发现双齿碳酸盐(b-CO₃²⁻)倾向于占据金属-半导体界面边缘位点，竞争性消耗*H吸附位点并改变析氢能垒。通过建立简化几何模型量化颗粒尺寸、活性位点比例与CO₂引起的产氢变化之间的关系，验证了b-CO₃²⁻的位点阻塞效应在Rh负载催化剂上占主导地位。通过调控Rh纳米颗粒尺寸可优化边缘位点比例，从而实现*H覆盖度与CO₂活化之间的平衡，促进CO₂RR生成甲烷。本研究通过边缘活性位点调控初步揭示了HER与CO₂RR的界面竞争机制，为催化剂的合理设计提供新见解，并为提升CO₂转化效率提供潜在策略。

关键词: 光热催化, 析氢, 二氧化碳还原, 活性位点, 界面竞争

Abstract:

Solar-driven photothermal catalytic CO₂ conversion with H₂O is a promising approach to produce sustainable fuels and chemicals. However, the competition between hydrogen evolution reaction (HER) and CO₂ reduction reaction (CO₂RR) results in unsatisfactory product selectivity. Noble metal nanoparticles (NMNPs) are widely used cocatalysts to introduce active sites on semiconductors, with unique active sites at the metal-semiconductor interfacial edges playing a critical role in the competitive mechanisms. Herein, we prepared a series of NMNPs loaded on Al-doped SrTiO₃ with abundant interfacial edge sites for continuous photothermal catalytic CO₂ and H₂O conversion. Different NMNPs demonstrated distinct CO₂-induced effects on hydrogen evolution. The key intermediate interactions were investigated by in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations. The results revealed that bidentate carbonate (b-CO₃²⁻) tended to occupy the edge sites at the metal-semiconductor interfaces, competitively consuming the active sites for *H adsorption and altering the energy barrier of hydrogen evolution. The predominant site-blocking effect of b-CO₃²⁻ on Rh-loaded catalysts was verified through establishing a simplified geometric model to quantify the correlation of particle sizes, active site proportions and CO₂-induced hydrogen production variations. Controlling Rh nanoparticle size can tune the proportion of edge sites, which involves a trade-off between *H coverage and CO₂ activation and promotes the CO₂RR process toward methane production. This work initially unravels the interfacial competitive mechanism between HER and CO₂RR via edge-active-site modulation, hoping to provide valuable insights for the rational catalyst design and offer potential strategies to enhance CO₂ conversion efficiency.

Key words: Photothermal catalysis, Hydrogen evolution, CO₂ reduction, Active site, Interfacial competition

洪佳楠, 许辰宇, 刘烟, 黎昌棋, 王梦琳, 张彦威. 通过边缘活性位点调控解析光热催化中析氢与二氧化碳还原的界面竞争[J]. 物理化学学报, 2025, 41(9), 100099. doi: 10.1016/j.actphy.2025.100099

Jianan Hong, Chenyu Xu, Yan Liu, Changqi Li, Menglin Wang, Yanwei Zhang. Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis[J]. Acta Phys. -Chim. Sin. 2025, 41(9), 100099. doi: 10.1016/j.actphy.2025.100099

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100099

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I9/100099

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通过边缘活性位点调控解析光热催化中析氢与二氧化碳还原的界面竞争

Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis

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通过边缘活性位点调控解析光热催化中析氢与二氧化碳还原的界面竞争

Decoding the interfacial competition between hydrogen evolution and CO2 reduction via edge-active-site modulation in photothermal catalysis

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Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis