Wenjing Ji, Hongtao Xie, Bangwei Deng, Yangyang Yu, Qin Geng, Yali Cao, Yizhao Li
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引用次数: 0
摘要
将二氧化碳(CO2)选择性光还原为甲烷(CH4)仍是一项重大挑战,其中涉及八个质子和八个电子的不利动力学转移。本文采用光沉积策略,在花状 Nb2O5 微球(Cu/Nb2O5)上沉积纳米铜金属,在模拟阳光下进行 CO2 光还原生成 CH4。结果表明,在不使用牺牲剂和光敏剂的情况下,1.0% Cu/Nb2O5 催化剂产生 CH4 的电子选择性为 84.8%,形成率为 15.89 μmol g-1 h-1。在 CO2 光还原过程中,1.0% Cu/Nb2O5 催化剂上 *CH3O 的生成是通过原位傅立叶变换红外光谱进行监测的。理论计算进一步表明,高稳定性 C1 中间体的形成在决定反应选择性方面起着至关重要的作用。通过优化催化剂的电子结构,该策略为 CO2 和 H2O 光催化转化为 CH4 产物提供了一种可行的策略,为开发高效、可持续的 CO2 转化技术提供了新的思路。此外,它还为光催化还原二氧化碳在温室气体减排和绿色能源生产中的广泛应用提供了有力的理论支持和实验依据。
Cu Metal-Modified Nb2O5 Microspheres Boost Photoreduction of CO2 to CH4 via Enhanced Adsorption of C1 Intermediates
Selective photoreduction of carbon dioxide (CO2) to methane (CH4) remains a major challenge, which involves a kinetically unfavorable transfer of eight protons and eight electrons. Herein, a photodeposition strategy was employed to deposit nano Cu metal on flower-like Nb2O5 microspheres (Cu/Nb2O5) for CO2 photoreduction to generate CH4 under simulated sunlight. The results show that the 1.0% Cu/Nb2O5 catalyst produces CH4 with an electron selectivity of 84.8% and a formation rate of 15.89 μmol g–1 h–1 without the use of sacrificial agents and photosensitizers. The generation of *CH3O on the 1.0% Cu/Nb2O5 catalyst during the CO2 photoreduction process was monitored using in situ Fourier transform infrared spectroscopy. Theoretical calculations further indicate the formation of highly stable C1 intermediates plays a crucial role in determining the reaction selectivity. By optimizing the electronic structure of the catalyst, this strategy provides a viable strategy for the photocatalytic conversion of CO2 and H2O into CH4 products, offering new insights into the development of efficient and sustainable CO2 conversion technologies. Moreover, it provides strong theoretical support and an experimental basis for the widespread application of photocatalytic CO2 reduction in greenhouse gas emission reduction and green energy production.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.