Journal ArticleDOI
Reduction of CO2 to CO by an Iron Porphyrin Catalyst in the Presence of Oxygen
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TLDR
In this article, an iron porphyrin complex with four ferrocene groups in its distal site is demonstrated to reduce CO2 unabated in the presence of O2 as it can reduce O2 to benign H2O under the same conditions.Abstract:
Reduction of CO2 to value-added chemicals is a logical way of fixing the rising levels of CO2. Activation and reduction of CO2 requires low-valent transition metals as catalysts. A major challenge in this chemistry is sensitivity of these low-valent metal sites to more abundant O2. Since O2 is a stronger oxidant than CO2 and isolated from the obvious competitive inhibition of CO2, partial reduction of O2 leads to formation of reactive oxygen species like O2– and H2O2, which are deleterious to the catalyst itself. An iron porphyrin complex appended with four ferrocene groups in its distal site is demonstrated to reduce CO2 unabated in the presence of O2 as it can reduce O2 to benign H2O under the same conditions. Further investigations reveal that iron porphyrins, in general, reduce CO2 selectively in the presence of O2. The aforementioned selectivity is derived from a 500 times faster rate of reaction of CO2 with Fe(0) porphyrin relative to O2 despite a higher driving force for the latter.read more
Citations
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Journal ArticleDOI
Advanced Electrocatalysts with Single-Metal-Atom Active Sites.
Yuxuan Wang,Hongyang Su,Yanghua He,Ligui Li,Shangqian Zhu,Hao Shen,Pengfei Xie,Xianbiao Fu,Guangye Zhou,Chen Feng,Dengke Zhao,Fei Xiao,Xiaojing Zhu,Yachao Zeng,Minhua Shao,Shaowei Chen,Gang Wu,Jie Zeng,Chao Wang +18 more
TL;DR: This review aims to provide a comprehensive summary on the recent development of single-atom electrocatalysts for various energy-conversion reactions using state-of-the-art microscopic and spectroscopic techniques.
Journal ArticleDOI
Porphyrin-based frameworks for oxygen electrocatalysis and catalytic reduction of carbon dioxide
TL;DR: Porphyrin-based frameworks, as specific kinds of metal-organic frameworks (MOFs) and covalent organic frameworks (COFs), have been widely used in energy-related conversion processes, including the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and also in energy related storage technologies such as rechargeable Zn-air batteries as discussed by the authors.
Journal ArticleDOI
Transition Metal Complexes as Catalysts for the Electroconversion of CO 2 : An Organometallic Perspective
TL;DR: In this paper, the authors cover selected examples to illustrate and categorize the currently favored mechanisms for the electrochemically induced transformation of CO2 promoted by homogeneous transition metal complexes and corroborate with the concepts and elementary steps of organometallic catalysis to derive potential strategies to broaden the molecular diversity of possible products.
Journal ArticleDOI
Recent advances in metalloporphyrin-based catalyst design towards carbon dioxide reduction: from bio-inspired second coordination sphere modifications to hierarchical architectures
TL;DR: This review collects the recent advances centred around the chemistry of metalloporphyrins for the reduction of CO2.
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Enabling storage and utilization of low-carbon electricity: power to formic acid
TL;DR: In this paper, a review of catalytic and heterogeneous catalysts for CO2 hydrogenation is presented, and an analysis for practical applications from the engineering viewpoint is provided with concluding remarks and an outlook for future challenges and R&D directions.
References
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Journal ArticleDOI
Catalysis of the electrochemical reduction of carbon dioxide
TL;DR: The general trends that transpire presently and are likely to be the object of active future work emphasis is put on the favorable role of acid addition in homogeneous catalytic systems and on the crucial chemical role of the electrode material in heterogeneous catalysis.
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A local proton source enhances CO2 electroreduction to CO by a molecular Fe catalyst.
TL;DR: Modification of iron tetraphenylporphyrin through the introduction of phenolic groups in all ortho and ortho′ positions of the phenyl groups considerably speeds up catalysis of this reaction by the electrogenerated iron(0) complex.
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Energy-Related Small Molecule Activation Reactions: Oxygen Reduction and Hydrogen and Oxygen Evolution Reactions Catalyzed by Porphyrin- and Corrole-Based Systems
TL;DR: Because of the significance of energy-related small molecule activation, this review covers recent progress in hydrogen evolution, oxygen evolution, and oxygen reduction reactions catalyzed by porphyrins and corroles.
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Visible-light-driven methane formation from CO 2 with a molecular iron catalyst
TL;DR: It is shown that an iron tetraphenylporphyrin complex functionalized with trimethylammonio groups, which is the most efficient and selective molecular electro- catalyst for converting CO2 to CO known, can also catalyse the eight-electron reduction ofCO2 to methane upon visible light irradiation at ambient temperature and pressure.
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Through-Space Charge Interaction Substituent Effects in Molecular Catalysis Leading to the Design of the Most Efficient Catalyst of CO2-to-CO Electrochemical Conversion.
TL;DR: The climax of this strategy of catalysis boosting by means of Coulombic stabilization of the initial Fe0-CO2 adduct is reached when four positively charged trimethylanilinium groups are introduced at the ortho positions of the TPP phenyls.