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Constructing Robust Bi Active Sites In Situ on α-Bi2O3 for Efficient and Selective Photoreduction of CO2 to CH4 via Directional Transfer of Electrons
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-02-03 , DOI: 10.1021/acscatal.2c05724
Weili Dai 1 , Ping Wang 1 , Jianfei Long 1 , Yong Xu 1 , Man Zhang 1 , Lixia Yang 1 , Jianping Zou 1 , Xubiao Luo 1 , Shenglian Luo 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-02-03 , DOI: 10.1021/acscatal.2c05724
Weili Dai 1 , Ping Wang 1 , Jianfei Long 1 , Yong Xu 1 , Man Zhang 1 , Lixia Yang 1 , Jianping Zou 1 , Xubiao Luo 1 , Shenglian Luo 1
Affiliation
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Photocatalytic CO2 reduction is an ideal strategy to reduce greenhouse effects and realize carbon neutralization. Constructing active sites with specific designs is highly desired and challenging to achieve with high activity and selectivity of photoreduction. Herein, our studies find that a series of Bi-based materials with different compositions, structures, and morphologies can be prepared by adjusting the pH. At pH 12.5, Bi nanocluster (NC)-modified Bi2O3 (Bi NCs/Bi2O3) are obtained, and the active site has changed from O of Bi2O3 to Bi of Bi NCs. Experimental and theoretical analyses suggest that photogenerated electrons in Bi NCs/Bi2O3 efficiently and directionally transfer from Bi2O3 to Bi NCs. As an outcome, Bi NCs/Bi2O3 possess outstanding adsorption and activation capacity of CO2, it achieves 94.8% of selectivity for visible light-driven CO2 reduction to CH4. According to the number of transferred electrons, the catalytic activity of Bi NCs/Bi2O3 is an amazing 210 times that of pure Bi2O3. It was found that the intermediate of *CO at Bi sites tended to be hydrogenated to form *CHO species in thermodynamics, and the intermediates of *CHO and *CH2OH/*CH3OH further formed on Bi NCs/Bi2O3, thus generating CH4 as a product. Whereas the above process is difficult to occur on Bi2O3, because the *CO easily desorbs to form CO. The results demonstrate that the evolution of active sites successfully leads to the change of CO2 photoreduction pathway.
中文翻译：
在 α-Bi2O3 上原位构建稳健的双活性位点，通过电子定向转移将 CO2 高效选择性地光还原为 CH4
光催化CO 2还原是减少温室效应和实现碳中和的理想策略。构建具有特定设计的活性位点是非常需要和具有挑战性的，以实现光还原的高活性和选择性。在此，我们的研究发现，通过调节 pH 值可以制备一系列具有不同组成、结构和形貌的铋基材料。在pH 12.5时，得到Bi纳米团簇(NC)修饰的Bi 2 O 3 (Bi NCs/Bi 2 O 3 )，活性位点由Bi 2 O 3的O变为Bi NCs的Bi。实验和理论分析表明，Bi NCs/Bi 2中的光生电子O 3有效且定向地从Bi 2 O 3转移到Bi NCs。因此，Bi NCs/Bi 2 O 3具有出色的CO 2吸附和活化能力，在可见光驱动下将CO 2还原为CH 4的选择性达到94.8% 。根据转移电子数，Bi NCs/Bi 2 O 3的催化活性是纯Bi 2 O 3的惊人的210倍。发现*CO在Bi位的中间体在热力学上倾向于氢化形成*CHO物种，*CHO和*CH的中间体在Bi NCs/Bi 2 O 3上进一步形成2 OH/*CH 3 OH ，从而生成CH 4作为产物。而上述过程在Bi 2 O 3上很难发生，因为*CO很容易解吸形成CO。结果表明，活性位点的演变成功地导致了CO 2光还原途径的改变。
更新日期：2023-02-03
中文翻译：
在 α-Bi2O3 上原位构建稳健的双活性位点，通过电子定向转移将 CO2 高效选择性地光还原为 CH4
光催化CO 2还原是减少温室效应和实现碳中和的理想策略。构建具有特定设计的活性位点是非常需要和具有挑战性的，以实现光还原的高活性和选择性。在此，我们的研究发现，通过调节 pH 值可以制备一系列具有不同组成、结构和形貌的铋基材料。在pH 12.5时，得到Bi纳米团簇(NC)修饰的Bi 2 O 3 (Bi NCs/Bi 2 O 3 )，活性位点由Bi 2 O 3的O变为Bi NCs的Bi。实验和理论分析表明，Bi NCs/Bi 2中的光生电子O 3有效且定向地从Bi 2 O 3转移到Bi NCs。因此，Bi NCs/Bi 2 O 3具有出色的CO 2吸附和活化能力，在可见光驱动下将CO 2还原为CH 4的选择性达到94.8% 。根据转移电子数，Bi NCs/Bi 2 O 3的催化活性是纯Bi 2 O 3的惊人的210倍。发现*CO在Bi位的中间体在热力学上倾向于氢化形成*CHO物种，*CHO和*CH的中间体在Bi NCs/Bi 2 O 3上进一步形成2 OH/*CH 3 OH ，从而生成CH 4作为产物。而上述过程在Bi 2 O 3上很难发生，因为*CO很容易解吸形成CO。结果表明，活性位点的演变成功地导致了CO 2光还原途径的改变。
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