Bottom-Up Interfacial Design of Covalent Organic Frameworks for Highly Efficient and Selective Electrocatalysis of CO2,Advanced Materials

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Bottom-Up Interfacial Design of Covalent Organic Frameworks for Highly Efficient and Selective Electrocatalysis of CO2
Advanced Materials ( IF 27.4 ) Pub Date : 2022-08-07 , DOI: 10.1002/adma.202205186
Ting He ₁ , Chenhuai Yang ₂ , Yongzhi Chen ₁ , Ning Huang ₃ , Shuming Duan ₂ , Zhicheng Zhang ₂ , Wenping Hu _{2,

4} , Donglin Jiang _{1,

4}

Affiliation

Assembling molecular catalytic centers into crosslinked networks is widely used to fabricate heterogeneous catalysts but they often suffer loss in activity and selectivity accompanied by unclear causes. Here, a strategy for the construction of heterogeneous catalysts to induce activity and selectivity by bottom-up introduction of segregated electron-conduction and mass-transport interfaces into the catalytic materials is reported. The catalytic skeletons are designed to possess different π orderings for electron motion and the open channels are tailored to install finely engineered walls for mass transport, so that origins of activity and selectivity are correlated. The resultant covalent organic framework catalysts with ordered π skeletons and solvophobic pores increase activity by two orders of magnitude, enhance selectivity and energy efficiency by 70-fold, and broaden the voltage range, to promote CO₂ transformation under ambient conditions. The results open a way to precise interfacial design of actionable heterogeneous catalysts for producing feedstocks from CO₂.

中文翻译：

用于 CO2 高效选择性电催化的共价有机框架的自下而上界面设计

将分子催化中心组装成交联网络被广泛用于制造非均相催化剂，但它们经常遭受活性和选择性的损失，原因不明。在这里，报道了一种构建非均相催化剂的策略，通过自下而上将分离的电子传导和质量传输界面引入催化材料来诱导活性和选择性。催化骨架被设计为具有不同的电子运动 π 排序，并且开放通道被定制为安装精细设计的壁以进行质量传输，从而使活性和选择性的起源相关联。得到的具有有序 π 骨架和疏溶剂孔的共价有机骨架催化剂将活性提高了两个数量级，₂环境条件下的转化。_{该结果为从 CO 2}生产原料的可操作多相催化剂的精确界面设计开辟了道路。

更新日期：2022-08-07

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