Converting Light Energy to Chemical Energy: A New Catalytic Approach for Sustainable Environmental Remediation.
Converting Light Energy to Chemical Energy: A New Catalytic Approach for Sustainable Environmental Remediation.
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DOI：
10.1021/acsomega.6b00076
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发表时间：
2016-07-31
期刊：
影响因子：
4.1
通讯作者：
Knecht, Marc R.
中科院分区：
文献类型：
--
作者：
Nguyen, Michelle A.;Zahran, Elsayed M.;Wilbon, Azaan S.;Besmer, Alexander V.;Cendan, Vincent J.;Ranson, William A.;Lawrence, Randy L.;Cohn, Joshua L.;Bachas, Leonidas G.;Knecht, Marc R.
我们报告了一种合成方法，形成立方Cu 2 O/Pd复合结构，并证明其作为串联催化的光催化材料的用途。将Pd纳米粒子负载于Cu 2 O立方体上，研究了其串联催化多氯联苯还原脱卤反应的活性。随着Pd含量的增加，催化剂的颗粒形貌和催化性能逐渐改善。在不同的Pd量下制备材料，并证明了一系列串联催化反应性。H2是通过由CuO引发的光催化质子还原产生的，然后使用原位产生的H2进行Pd催化脱卤。结果表明，材料的形貌和组成以及底物的空间位阻效应在控制反应速率方面起着重要的作用。此外，对反应后材料的分析表明，在光脱氯反应期间，少量立方体已经变得中空。这些发现提供了关于光催化活性位点和机制的重要见解，为通常不通过光驱动的可持续催化反应提供了将光能转化为化学能的途径。
We report a synthetic approach to form cubic Cu2O/Pd composite structures and demonstrate their use as photocatalytic materials for tandem catalysis. Pd nanoparticles were deposited onto Cu2O cubes, and their tandem catalytic reactivity was studied via the reductive dehalogenation of polychlorinated biphenyls. The Pd content of the materials was gradually increased to examine its influence on particle morphology and catalytic performance. Materials were prepared at different Pd amounts and demonstrated a range of tandem catalytic reactivity. H2 was generated via photocatalytic proton reduction initiated by Cu2O, followed by Pd-catalyzed dehalogenation using in situ generated H2. The results indicate that material morphology and composition and substrate steric effects play important roles in controlling the overall reaction rate. Additionally, analysis of the postreacted materials revealed that a small number of the cubes had become hollow during the photodechlorination reaction. Such findings offer important insights regarding photocatalytic active sites and mechanisms, providing a pathway toward converting light-based energy to chemical energy for sustainable catalytic reactions not typically driven via light.
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