光化学H2解离近定量CO2还原为乙烯
近日,中国科学院大连化学物理研究所王峰团队实现了光化学H2解离近定量CO2还原为乙烯。该研究于2025年9月4日发表在《科学》杂志上。
通过二氧化碳(CO2)加氢生产烯烃是一个长期的目标。产物为多碳混合物,这是高温异氢解离反应的关键步骤,使选择性控制复杂化。
在这项工作中,研究组报道了在室温下辐照365纳米的金-二氧化钛诱导H2异解离解。这一过程可能依赖于位于金属金纳米颗粒和界面金氧钛支架上的光生电子和空穴产生的界面电偶极子。在金纳米粒子表面包覆氧化钛层,进一步促进了氢的异解离解。在流动装置的光照射下,产生的亲核氢以99%的收率将CO2还原为乙烷。此外,与随后的光催化乙烷脱氢级联,在1500小时的辐照下,乙烯的产率达到99%。
附:英文原文
Title: Photochemical H2 dissociation for nearly quantitative CO2 reduction to ethylene
Author: Ping Jin, Pu Guo, Nengchao Luo, Hui Zhang, Chenwei Ni, Ruotian Chen, Wei Liu, Rengui Li, Jianping Xiao, Guoxiong Wang, Fuxiang Zhang, Paolo Fornasiero, Feng Wang
Issue&Volume: 2025-09-04
Abstract: Producing olefins by carbon dioxide (CO2) hydrogenation is a long-standing goal. The usual products are multicarbon mixtures because the critical step of heterolytic hydrogen (H2) dissociation at high temperatures complicates selectivity control. In this study, we report that irradiating gold–titanium dioxide at 365 nanometers induces heterolytic H2 dissociation at ambient temperature. This process likely relies on interfacial electric dipoles from photogenerated electrons and holes situated on the metallic gold nanoparticles and interfacial gold–oxygen–titanium scaffolds. The heterolytic H2 dissociation is further promoted by light-induced coating of gold nanoparticles with a titanium oxide layer. The resulting nucleophilic hydrogen species reduce CO2 to ethane in >99% yield under light irradiation in a flow apparatus. Furthermore, cascading with a subsequent photocatalytic ethane dehydrogenation generates ethylene in >99% yield over 1500 hours of irradiation.
DOI: adq3445
Source: https://www.science.org/doi/10.1126/science.adq3445