The Promotional Effects of Heteroatom Doping and Alloy Nanoparticle Confinement
The Promotional Effects of Heteroatom Doping and Alloy Nanoparticle Confinement
复制标题
杂原子掺杂和合金纳米粒子限制的促进作用
DOI：
10.1021/acsaem.1c02369
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发表时间：
2021
影响因子：
6.4
通讯作者：
H. Yamashita
中科院分区：
文献类型：
--
作者：
K. Mori;J. Matsuo;Y. Kondo;H. Hata;H. Yamashita
开发具有高活性的光催化体系来引发CO2还原成甲酸（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一个有吸引力的选择。研究了杂原子掺杂以及Pd合金纳米颗粒（NPs）对胺功能化的铁基金属有机骨架（Fe 3-MOF）的限制作用。金属簇节点中不同金属的取代显著改变了CO2吸附容量以及可见光照射下的CO2活化性能，其中Mn 2+掺杂尤其改善了两者的性能。PdAu NPs的限制通过有效地捕获激发电子来抑制电子-空穴复合，然后促进光催化FA的产生。通过优化工艺参数，在24 h后，FA产量可达725 μmol·g-1，是未改性Fe 3-MOF的3.6倍。本研究的结果有可能大大丰富的应用MOF基光催化剂的目的是开发经济的CO2介导的储氢能量循环。
The development of photocatalytic systems with high activity to trigger CO2reduction 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 CO2adsorption capacity as well as the CO2activation 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–1can 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.