Citation: Yuehan Cao, Rui Guo, Minzhi Ma, Zeai Huang, Ying Zhou. Effects of Electron Density Variation of Active Sites in CO₂ Activation and Photoreduction: A Review[J]. Acta Physico-Chimica Sinica, ;2024, 40(1): 230302. doi: 10.3866/PKU.WHXB202303029 shu

Effects of Electron Density Variation of Active Sites in CO₂ Activation and Photoreduction: A Review

Yuehan Cao ^{1, 2, †} ,
Rui Guo ^{2, †} ,
Minzhi Ma ² ,
Zeai Huang ² ,
Ying Zhou ^{1, 2,,}

1.
State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China
2.
School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China

Corresponding author: Ying Zhou, yzhou@swpu.edu.cn

^†

Received Date: 14 March 2023
Revised Date: 13 April 2023
Accepted Date: 14 April 2023
Available Online: 20 April 2023
Fund Project: the National Natural Science Foundation of China 22209135Special Project for the Central Government to Guide the Development of Local Science and Technology in Sichuan Province 22ZYZYTS0231China Postdoctoral Science Foundation 2022M722635Natural Science Foundation of Sichuan Province 2022NSFSC1264Sichuan Science and Technology Program 2021ZYD0035Sichuan Science and Technology Program 2022YFH0084Sichuan Science and Technology Program 2021YFH0055Sichuan Science and Technology Program 2022YFSY0050

Photocatalytic reduction of CO₂ into value-added chemicals is a feasible approach to harvest solar light energy and storing energy in the form of chemical fuels as well as to mitigate the effects of global climate change and help achieve an artificial carbon cycle. However, the efficiency of CO₂ photoreduction is low for commercial purposes. This is mainly due to the difficult adsorption and activation process of CO₂ molecules, the unsatisfactory selectivity of target products, and the uncontrolled-subsequent reaction process of the generated carbon products. CO₂ photoreduction requires substantial electrons for participation. Hence, these issues are due to the electron density modulation of the active sites of catalysts. Unfortunately, the CO₂ photoreduction process involves multi-fundamental steps, which leads to different requirements in electron density modulation. The performance might not be effectively improved by directly enhancing or weakening the total electron density of active sites. In this paper, we summarize recent advances in the influence of electron density variation of the active sites in strengthening the adsorption and activation of CO₂ molecules, enhancing the selectivity of target carbon products and modulating the subsequent reaction process of the generated carbon products. This review begins with the effect of different types of active sites in strengthening the adsorption and activation of the CO₂ molecules and the related methods for modulating the electron density of active sites. Active sites with high electron densities can significantly enhance the adsorption and activation of CO₂. Introducing metal and fabricating the defects on catalyst surfaces are effective strategies for fabricating the electron-rich active sites. After that, we discuss the influence of electron density variation in enhancing the selectivity of target carbon products in detail. In this part, the related effects in the multielectron donation from the catalyst surface, the reactive intermediates, and the competition hydrogen evolution reaction are summarized. Enhancing the electron density of active sites strengthens the former two processes. For multielectron donation, introducing cocatalysts or fabricating heterostructures are the most effective methods for enhancing the electron density of active sites. The adsorption and conversion process of intermediates are mainly affected by the accumulation sites of electrons. The active sites with low coordination are more favorable to achieving the generation of multi-electronic carbon products. In contrast, the hydrogen evolution reaction is significantly inhibited by reducing the electron density of active sites. Moreover, elemental doping is considered one of the most effective strategies. Finally, we describe the method for weakening the electron density of active sites to promote product desorption and inhibit the photooxidation of reactive products.
- CO₂ photoreduction,
- Value-added chemicals,
- Electron density modulation,
- Active sites,
- Product selectivity
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Effects of Electron Density Variation of Active Sites in CO2 Activation and Photoreduction: A Review

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Effects of Electron Density Variation of Active Sites in CO₂ Activation and Photoreduction: A Review