Boosting Photocatalytic CO2 Reduction on CsPbBr3 Perovskite Nanocrystals by Immobilizing Metal Complexes
Boosting Photocatalytic CO2 Reduction on CsPbBr3 Perovskite Nanocrystals by Immobilizing Metal Complexes
复制标题
通过固定金属配合物促进 CsPbBr3 钙钛矿纳米晶体光催化 CO2 还原
DOI：
10.1021/acs.chemmater.9b04582
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发表时间：
2020-02-25
影响因子：
8.6
通讯作者：
Gaponik, Nikolai
中科院分区：
文献类型：
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作者：
Chen, Zhoujie;Hu, Yangguang;Gaponik, Nikolai
利用光催化剂和阳光将二氧化碳转化为化学燃料是解决气候恶化和能源危机的一种有吸引力的方法。金属配合物因其具有高活性的可调催化位点而成为二氧化碳减排的绝佳候选者。金属配合物与有机光敏剂的偶联被认为是建立可见光驱动的二氧化碳还原光催化系统的常用策略。虽然大多数有机光敏剂通常含有贵金属并且可以通过繁琐的合成路线获得，但它们在光催化中的大规模应用受到限制。卤化物钙钛矿纳米晶（NC）由于其光吸收范围可调、成本低、表面位点丰富和摩尔消光系数高而被认为是最有前途的替代有机光敏剂的光捕获材料之一。在此，我们展示了一种简单的策略，将 [Ni(terpy)(2)](2+) (Ni(tpy)) 固定在无机配体封端的 CsPbBr3 NC 上，并将这种杂化物用作可见光驱动的 CO2 还原的催化剂。在这种混合光催化系统中，Ni(tpy)可以提供特定的催化位点并充当电子汇以抑制CsPbBr3 NC中的电子空穴复合。 CsPbBr3-Ni(tpy)催化系统在将CO2还原为CO/CH4时实现了高产率（1724 μmol/g），比原始CsPbBr3 NCs高出约26倍。这项工作开发了一种通过将金属配合物固定在钙钛矿纳米颗粒上来增强光催化二氧化碳还原性能的方法。我们在此介绍的方法为利用卤化物钙钛矿纳米颗粒进行光催化应用提供了一个新平台。
Converting CO2 into chemical fuels with a photocatalyst and sunlight is an appealing approach to address climate deterioration and energy crisis. Metal complexes are superb candidates for CO2 reduction due to their tunable catalytic sites with high activity. The coupling of metal complexes with organic photosensitizers is regarded as a common strategy for establishing photocatalytic systems for visible-light-driven CO2 reduction. While most of the organic photosensitizers generally contain precious metals and are available through onerous synthetic routes, their large-scale application in the photocatalysis is limited. Halide perovskite nanocrystals (NCs) have been considered as one of the most promising light-harvesting materials to replace the organic photosensitizers due to their tunable light absorption range, low cost, abundant surface sites, and high molar extinction coefficient. Herein, we demonstrate a facile strategy to immobilize [Ni(terpy)(2)](2+) (Ni(tpy)) on inorganic ligand-capped CsPbBr3 NCs and to apply this hybrid as a catalyst for visible-light-driven CO2 reduction. In this hybrid photocatalytic system, the Ni(tpy) can provide specific catalytic sites and serve as electron sinks to suppress electron hole recombination in the CsPbBr3 NCs. The CsPbBr3-Ni(tpy) catalytic system achieves a high yield (1724 mu mol/g) in the reduction of CO2 to CO/CH4, which is approximately 26-fold higher than that achieved with the pristine CsPbBr3 NCs. This work has developed a method for enhancing the performance of photocatalytic CO2 reduction by immobilizing metal complexes on perovskite NCs. The methodology we present here provides a new platform for utilizing halide perovskite NCs for photocatalytic applications.