Decoration of Active Sites in Covalent–Organic Framework: An Effective Strategy of Building Efficient Photocatalysis for CO2 Reduction,ACS Sustainable Chemistry & Engineering

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Decoration of Active Sites in Covalent–Organic Framework: An Effective Strategy of Building Efficient Photocatalysis for CO2 Reduction
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-09-20 , DOI: 10.1021/acssuschemeng.1c04994
Yan Yang ₁ , Yang Lu ₁ , Hong-Yu Zhang ₁ , Ya Wang ₁ , Hong-Liang Tang ₁ , Xiao-Jun Sun ₁ , Guiling Zhang ₁ , Feng-Ming Zhang ₁

Affiliation

The decoration of metal active sites to realize the regulation of catalytic activity of photocatalysts is greatly meaningful. Here, we rationally tune the coordination environment of metal centers in covalent–organic framework (COF) for efficient photocatalytic CO₂ reduction. 3,3′,5,5′-Tetraformyl-4,4′-biphenyldiol-COF (TFBD-COF) was synthesized and then used for immobilizing Co²⁺, followed by the coordination of salicylideneaniline (SA) ligand to construct TFBD-COF-Co-SA that shows excellent photocatalytic CO₂ reduction activity and stability. As a result, TFBD-COF-Co-SA shows a CO₂-to-CO reduction activity of 7400 μmol·g^–1 in 5 h and a 90% selectivity. Different from simply coordinating metal ions to COFs, the CO evolution rate of TFBD-COF-Co-SA is 4.1 times higher than that of TFBD-COF-Co without the coordination of SA ligand. It is confirmed that this heterocatalytic activity of TFBD-COF-Co-SA is comparable to the homocatalytic activity of the Co(SA)₂ complex molecular catalyst calculated on the basis of the number of metal centers.

中文翻译：

共价有机框架中活性位点的装饰：构建高效光催化二氧化碳还原的有效策略

金属活性位点的修饰实现对光催化剂催化活性的调控意义重大。在这里，我们合理调整共价有机骨架（COF）中金属中心的配位环境，以实现高效的光催化 CO ₂还原。合成3,3',5,5'-Tetraformyl-4,4'-联苯二醇-COF (TFBD-COF)，然后用于固定Co ²⁺，然后配位水杨基苯胺(SA)配体构建TFBD- COF-Co-SA 具有优异的光催化 CO ₂还原活性和稳定性。因此，TFBD-COF-Co-SA 的 CO ₂ -CO 还原活性为 7400 μmol·g ^–1在 5 小时内，选择性为 90%。与简单地将金属离子配位至 COF 不同，TFBD-COF-Co-SA 的 CO 析出速率比没有配位 SA 配体的 TFBD-COF-Co 高 4.1 倍。证实TFBD-COF-Co-SA的这种杂催化活性与基于金属中心数计算的Co(SA) ₂复合分子催化剂的均催化活性相当。

更新日期：2021-10-04

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