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Multielectron transportation of polyoxometalate-grafted metalloporphyrin coordination frameworks for selective CO2-to-CH4 photoconversion
National Science Review ( IF 20.6 ) Pub Date : 2019-07-16 , DOI: 10.1093/nsr/nwz096
Qing Huang 1 , Jiang Liu 1 , Liang Feng 2 , Qi Wang 3 , Wei Guan 3 , Long-Zhang Dong 1 , Lei Zhang 1 , Li-Kai Yan 3 , Ya-Qian Lan 1 , Hong-Cai Zhou 2
Affiliation  

Photocatalytic CO2 reduction into energy carriers is of utmost importance due to the rising concentrations of CO2 and the depleting energy resource. However, the highly selective generation of desirable hydrocarbon fuel, such as methane (CH4), from CO2 remains extremely challenging. Herein, we present two stable polyoxometalate-grafted metalloporphyrin coordination frameworks (POMCFs), which are constructed with reductive Zn-ϵ-Keggin clusters and photosensitive tetrakis(4-carboxylphenyl)porphyrin (H2TCPP) linkers, exhibiting high selectivity (>96%) for CH4 formation in a photocatalytic CO2-reduction system. To our knowledge, the high CH4 selectivity of POMCFs has surpassed all of the reported coordination-framework-based heterogeneous photocatalysts for CO2-to-CH4 conversion. Significantly, the introduction of a Zn-ϵ-keggin cluster with strong reducing ability is the important origin for POMCFs to obtain high photocatalytic selectivity for CH4 formation, considering that eight MoV atoms can theoretically donate eight electrons to fulfill the multielectron reduction process of CO2-to-CH4 transformation.

中文翻译:

多金属氧酸盐接枝金属卟啉配位框架的多电子传输,用于选择性 CO2 至 CH4 光转化

由于CO 2浓度升高和能源消耗,光催化CO 2还原为能量载体是最重要的。然而,从 CO 2高度选择性地产生所需的碳氢化合物燃料,例如甲烷 (CH 4 )仍然极具挑战性。在此,我们提出了两种稳定的多金属氧酸盐接枝金属卟啉配位框架 (POMCFs),它们由还原性 Zn-ϵ-Keggin 簇和光敏四 (4-羧基苯基)卟啉 (H 2 TCPP) 连接器构建,表现出高选择性 (>96%) )在光催化 CO 2还原系统中形成CH 4。据我们所知,高 CH 4POMCFs 的选择性已经超过了所有报道的基于协调框架的多相光催化剂用于 CO 2到 CH 4 的转化。值得注意的是,考虑到 8 个 Mo V原子理论上可以提供 8 个电子来完成多电子还原过程,因此引入具有强还原能力的 Zn-ϵ-keggin 簇是 POMCFs 获得高光催化 CH 4选择性的重要来源。 CO 2到CH 4 的转化。
更新日期:2020-04-17
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