Photochemical H2 dissociation for nearly quantitative CO2 reduction to ethylene

• 成果类型: Article
• 署名作者: Jin, Ping; Guo, Pu; Luo, Nengchao; Zhang, Hui; Ni, Chenwei; Chen, Ruotian; Liu, Wei; Li, Rengui; Xiao, Jianping; Wang, Guoxiong; Zhang, Fuxiang; Fornasiero, Paolo; Wang, Feng
• 署名单位: Chinese Academy of Sciences; Dalian Institute of Chemical Physics, CAS; Chinese Academy of Sciences; University of Chinese Academy of Sciences, CAS; Chinese Academy of Sciences; Shanghai Advanced Research Institute, CAS; Chinese Academy of Sciences; Shanghai Institute of Microsystem & Information Technology, CAS; Fudan University; University of Trieste; University of Trieste; Consiglio Nazionale delle Ricerche (CNR); Isituto di Chimica dei Composti Organometallici (ICCOM-CNR)
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8075; 1095-9203
• DOI: 10.1126/science.adq3445
• 发表日期: 2025-09-04
• 页码: 1037-1042
• 关键词: ELASTIC BAND METHOD; photocatalytic reduction; gold nanoparticles; AU NANOPARTICLES; particle-size; tio2; conversion; energy; water; hydrogenation

摘要

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 (H-2) dissociation at high temperatures complicates selectivity control. In this study, we report that irradiating gold-titanium dioxide at 365 nanometers induces heterolytic H-2 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 H-2 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.