Photochemical H2 dissociation for nearly quantitative CO2 reduction to ethylene

IF 45.8 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Pub Date : 2025-09-04 DOI:10.1126/science.adq3445

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

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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.

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光化学H2解离近定量CO2还原为乙烯

通过二氧化碳（CO2）加氢生产烯烃是一个长期的目标。通常的产物是多碳混合物，因为高温下杂解氢（H2）解离的关键步骤使选择性控制复杂化。在这项研究中，我们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小时的照射下，乙烯的收率为99%。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science 综合性期刊-综合性期刊

CiteScore

61.10

自引率

0.90%

发文量

审稿时长

2.1 months

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