南京师范大学刘犇团队报道了可调多元金属有机框架作为光催化剂设计平台。相关研究成果发表在2021年4月26日出版的《美国化学会杂志》。

光化学反应的催化剂是我们生活中许多基础的基础，例如，从自然采光到现代能量储存和转换，包括二氧化钛的水光解等过程。近年来，金属-有机框架（MOF）因其结构多样性和可调性在设计光催化剂以应对能源和环境挑战方面的优势而引起了化学研究界的广泛关注。

该文中，研究人员报道了一系列新的多元金属-有机框架（MTV-MOFs），表示为MTV-MIL-100。它们是由芳香羧酸盐和具有有序原子排列的AB2OX3双金属团簇连接而成。通过溶剂辅助的方法合成，这些有序和多元的金属团簇提供了一个增强和微调晶体材料的电子结构的机会来。此外，利用MOF结构的高孔隙率提高了传质性能。结合这些主要优点，MTV-MIL-100（Ti，Co）在氨硼烷光催化水解中具有高的光活性，其周转率为113.7molH2 gcat.^–1min^–1，量子效率为4.25%，时空产率为4.96× 10^-5。

该研究工作架起了钙钛矿和MOFs的桥梁，为高活性光催化剂的设计提供了一个新的平台。

附：英文原文

Title: A Tunable Multivariate Metal–Organic Framework as a Platform for Designing Photocatalysts

Author: Yang Wang, Hao Lv, Erik Svensson Grape, Carlo Alberto Gaggioli, Akhil Tayal, Aditya Dharanipragada, Tom Willhammar, A. Ken Inge, Xiaodong Zou, Ben Liu, Zhehao Huang

Issue&Volume: April 26, 2021

Abstract: Catalysts for photochemical reactions underlie many foundations in our lives, from natural light harvesting to modern energy storage and conversion, including processes such as water photolysis by TiO2. Recently, metal–organic frameworks (MOFs) have attracted large interest within the chemical research community, as their structural variety and tunability yield advantages in designing photocatalysts to address energy and environmental challenges. Here, we report a series of novel multivariate metal–organic frameworks (MTV-MOFs), denoted as MTV-MIL-100. They are constructed by linking aromatic carboxylates and AB2OX3 bimetallic clusters, which have ordered atomic arrangements. Synthesized through a solvent-assisted approach, these ordered and multivariate metal clusters offer an opportunity to enhance and fine-tune the electronic structures of the crystalline materials. Moreover, mass transport is improved by taking advantage of the high porosity of the MOF structure. Combining these key advantages, MTV-MIL-100(Ti,Co) exhibits a high photoactivity with a turnover frequency of 113.7 molH2 gcat.–1 min–1, a quantum efficiency of 4.25%, and a space time yield of 4.96 × 10–5 in the photocatalytic hydrolysis of ammonia borane. Bridging the fields of perovskites and MOFs, this work provides a novel platform for the design of highly active photocatalysts.

DOI: 10.1021/jacs.1c01764

Source: https://pubs.acs.org/doi/10.1021/jacs.1c01764