A Highly Durable, Self-Photosensitized Mononuclear Ruthenium Catalyst for CO2 Reduction

A Highly Durable, Self-Photosensitized Mononuclear Ruthenium Catalyst for CO2 Reduction
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用于二氧化碳还原的高度耐用、自光敏单核钌催化剂

DOI:
10.1055/a-1709-0280
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发表时间:
2021
期刊:
影响因子:
2
通讯作者:
Morikawa Takeshi
Morikawa Takeshi
中科院分区:
化学4区
文献类型:
--
作者:
Jung Jieun;Saito Susumu;Kamada Kenji;Okuwa Hiroko;Wakabayashi Taku;Sekizawa Keita;Sato Shunsuke;Morikawa Takeshi

文献摘要

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一种新型的单核钌(Ru)配合物轴承PNNP型四齿配体在这里介绍作为一种自光敏催化剂,用于还原二氧化碳(CO2)。当钌配合物通过与碱的反应进行预活化时,催化剂的诱导期几乎消失,并且在144 h的反应时间内催化剂周转数(TONs)分别达到307和489,对于一氧化碳(CO)和甲酸(HCO2H)。该配合物具有长寿命的双重光敏剂和还原催化剂,由于空间庞大和结构稳健(PNNP)Ru框架。在13CO2气氛下的同位素标记实验表明,CO和HCO2H都是由CO2产生的。
A novel mononuclear ruthenium (Ru) complex bearing a PNNP-type tetradentate ligand is introduced here as a self-photosensitized catalyst for the reduction of carbon dioxide (CO2). When the pre-activation of the Ru complex by reaction with a base was carried out, an induction period of catalyst almost disappeared and the catalyst turnover numbers (TONs) over a reaction time of 144 h reached 307 and 489 for carbon monoxide (CO) and for formic acid (HCO2H), respectively. The complex has a long lifespan as a dual photosensitizer and reduction catalyst, due to the sterically bulky and structurally robust (PNNP)Ru framework. Isotope-labeling experiments under13CO2atmosphere indicate that CO and HCO2H were both produced from CO2.