Immobilization of a Full Photosystem in the Large-Pore MIL-101 Metal-Organic Framework for CO2 reduction.
Immobilization of a Full Photosystem in the Large-Pore MIL-101 Metal-Organic Framework for CO2 reduction.
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DOI：
10.1002/cssc.201801066
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发表时间：
2018-08
期刊：
影响因子：
8.4
通讯作者：
Xia Wang;F. Wisser;J. Canivet;M. Fontecave;C. Mellot‐Draznieks
中科院分区：
文献类型：
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作者：
Xia Wang;F. Wisser;J. Canivet;M. Fontecave;C. Mellot‐Draznieks
通过简单的后合成浸渍，将分子催化剂 [Cp*Rh(4,4'-bpydc)]2+ 和分子光敏剂 [Ru(bpy)2 (4,4'-bpydc)]2+ (bpydc=联吡啶二甲酸)共固定到高度多孔的金属有机框架 MIL-101-NH2 (Al) 中。 Rh-Ru@MIL-101-NH2 复合材料可以在可见光下还原 CO2，同时通过独家生产甲酸盐表现出卓越的选择性。这种 Rh-Ru@MIL-101-NH2 固体代表了第一个以非共价方式用催化剂和光敏剂功能化 MOF 的例子。由于催化剂和光敏剂被共同限制在空腔的纳米空间中，MOF 孔被用作纳米反应器，并能够以非均相方式进行分子催化。
A molecular catalyst [Cp*Rh(4,4'-bpydc)]2+ and a molecular photosensitizer [Ru(bpy)2 (4,4'-bpydc)]2+ (bpydc=bipyridinedicarboxylic acid) were co-immobilized into the highly porous metal-organic framework MIL-101-NH2 (Al) upon easy postsynthetic impregnation. The Rh-Ru@MIL-101-NH2 composite allows the reduction of CO2 under visible light, while exhibiting remarkable selectivity with the exclusive production of formate. This Rh-Ru@MIL-101-NH2 solid represents the first example of MOFs functionalized with both a catalyst and a photosensitizer in a noncovalent fashion. Thanks to the coconfinement of the catalyst and photosensitizer into the cavity's nanospace, the MOF pores are used as nanoreactors and enable molecular catalysis in a heterogeneous manner.