Photoreduction of Carbon Dioxide to Formic Acid with Fe-Based MOFs: The Promotional Effects of Heteroatom Doping and Alloy Nanoparticle Confinement,ACS Applied Energy Materials

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Photoreduction of Carbon Dioxide to Formic Acid with Fe-Based MOFs: The Promotional Effects of Heteroatom Doping and Alloy Nanoparticle Confinement
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-09-21 , DOI: 10.1021/acsaem.1c02369
Kohsuke Mori _{1,

2,

3} , Jumpei Matsuo ₁ , Yoshifumi Kondo ₁ , Hiroto Hata ₁ , Hiromi Yamashita _{1,

2,

3}

Affiliation

The development of photocatalytic systems with high activity to trigger CO₂ reduction into formic acid (FA, HCOOH), which is regarded as a promising hydrogen storage compound, is an attractive option for simultaneously solving energy and environmental problems. The effects of heteroatom doping as well as the confinement of Pd alloy nanoparticles (NPs) on an amine-functionalized Fe-based metal organic framework (Fe₃-MOF) were investigated. The substitution of different metals in the metal cluster nodes significantly changed the CO₂ adsorption capacity as well as the CO₂ activation properties under visible light irradiation, with Mn²⁺ doping particularly improving the performance of both. The confinement of PdAu NPs inhibited electron–hole recombination by efficiently trapping excited electrons and then promoting photocatalytic FA production. By optimizing the parameters, a high FA production of 725 μmol·g^–1 can be achieved after 24 h, which is 3.6 times greater than that obtained with unmodified Fe₃-MOF. The results of the present study have the potential to greatly enrich the applications of MOF-based photocatalysts with the aim of developing economical CO₂-mediated hydrogen storage energy cycling.

中文翻译：

用铁基 MOF 将二氧化碳光还原为甲酸：杂原子掺杂和合金纳米粒子限制的促进作用

开发具有高活性的光催化体系以触发 CO ₂还原为甲酸（FA，HCOOH），甲酸被认为是一种有前途的储氢化合物，是同时解决能源和环境问题的有吸引力的选择。研究了杂原子掺杂的影响以及 Pd 合金纳米粒子 (NPs) 对胺功能化的 Fe基金属有机骨架 (Fe ₃ -MOF) 的限制。金属簇节点中不同金属的取代显着改变了可见光照射下的CO ₂吸附能力和CO ₂活化性能，Mn ²⁺兴奋剂尤其可以提高两者的性能。PdAu NPs 的限制通过有效地捕获激发的电子然后促进光催化 FA 的产生来抑制电子 - 空穴复合。通过优化参数，24 小时后可实现725 μmol·g ^–1的高 FA 产量，是未改性 Fe ₃ -MOF获得的产量的3.6 倍。本研究的结果有可能极大地丰富基于 MOF 的光催化剂的应用，旨在开发经济的 CO ₂介导的储氢能量循环。

更新日期：2021-10-25

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