Steering artificial photosynthesis via photoinduced conversion of monometallic to bimetallic sites in FeCo nitroprussides.

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Hao Wang, Gui-Lin Zhuang, Yingjie Fan, Hua-Qing Yin, Wei Zhang, Zhe Wu, Shuang Yao, Tong-Bu Lu, Wenbin Lin, Zhi-Ming Zhang
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引用次数: 0

Abstract

Artificial photosynthesis provides an efficient strategy for solar energy storage via water splitting and CO2 reduction, but it remains a challenge in tuning artificial photosynthesis between these two competing reactions. Herein, we demonstrate photoinduced conversion of monometallic to bimetallic sites in a Fe-Co nitroprusside (FeCo-NP) to steer the reaction path from H2 evolution to CO2 reduction. Monometallic Co sites achieve efficient H2 production with 28.5 mmol g-1 activity and 85.4% selectivity. Photoinduced release of nitrosyl groups from Fe sites generates bimetallic Fe-Co sites, which suppress H2 evolution and enhance CO2 reduction, yielding 31.5 mmol g-1 activity and 87.3% selectivity for C1 products. Mechanistic investigations reveal that monometallic Co sites catalyze H2 evolution via H2O adsorption and O-H cleavage while bimetallic Fe-Co sites facilitate both H2O and CO2 adsorption and subsequent O and C hydrogenation for CO and HCOOH. This work uncovers a strategy to manipulate competing reaction pathways via photoinduced conversion of monometallic to bimetallic sites, which provides unique insights into addressing environmental issues and energy crises.

通过光诱导将FeCo硝普苷中的单金属位转化为双金属位来引导人工光合作用。
人工光合作用通过水分解和二氧化碳还原为太阳能储存提供了有效的策略,但在这两个相互竞争的反应之间进行人工光合作用的调整仍然是一个挑战。在本研究中,我们展示了Fe-Co硝普苷(FeCo-NP)中单金属到双金属位点的光诱导转化,以引导从H2析出到CO2还原的反应路径。单金属Co位点的产氢效率为28.5 mmol g-1,选择性为85.4%。光诱导释放Fe位点的亚硝基生成双金属Fe- co位点,抑制H2的生成,增强CO2的还原能力,C1产物的活性为31.5 mmol g-1,选择性为87.3%。机制研究表明,单金属Co位点通过H2O吸附和O- h裂解催化H2的析出,而双金属Fe-Co位点同时促进H2O和CO2吸附以及Co和HCOOH的O和C加氢。这项工作揭示了一种通过光诱导将单金属转化为双金属位点来操纵竞争反应途径的策略,这为解决环境问题和能源危机提供了独特的见解。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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