Recent Progress in (Photo-)-Electrochemical Conversion of CO(2) With Metal Porphyrinoid-Systems.
Recent Progress in (Photo-)-Electrochemical Conversion of CO(2) With Metal Porphyrinoid-Systems.
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DOI：
10.3389/fchem.2021.685619
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发表时间：
2021
影响因子：
5.5
通讯作者：
Schöfberger W
中科院分区：
文献类型：
--
作者：
Dedić D;Dorniak A;Rinner U;Schöfberger W
几十年来，全球社会一直面临着环境危机，因此需要从过时的能源转向新的、更有效的能源，并以更有效的方式应对不断增加的二氧化碳排放。以低成本、低能耗的方式活化O2、H+和CO2等小分子已成为催化研究的关键课题之一。关于这些分子的活化的主要问题是为了使催化反应发生而必须克服的动力学障碍。大自然已经提供了许多途径，在这些途径中，小分子被激活并转化为具有更高能量水平的化合物。最著名的例子之一是光合作用，其中CO2通过阳光转化为葡萄糖和O2，从而将太阳能转化为化学能。自然界中的这些转化主要是利用酶作为催化剂进行的，其中卟啉和类卟啉结构的催化剂就存在于其中，因此设计新型的类卟啉体系成为研究的热点（例如钴、卟啉和酞菁），其金属配合物可用于将CO2直接电催化还原为有价值的化学物质，如一氧化碳、甲酸盐、甲醇、乙醇、甲烷、乙烯，或乙酸盐。例如，钴（III）三苯基膦咔咯络合物已被用作将CO2电还原为乙醇和甲醇的催化剂。该研究领域的总体目标和重点是开发一种工业用途的方法，提出了是否以及如何将催化剂结合到支持材料上的问题。氧化石墨烯、多壁碳纳米管、炭黑和活性炭，仅举几个例子，已经成为研究的选择。这些材料还通过例如防止竞争反应（例如CO2还原期间的析氢反应（HER））而对催化具有有益效果。很明显，小分子活化的主题为我们当前的能源和环境危机提供了许多解决方案，并正在成为一个深入研究的研究目标。这篇综述文章旨在概述最近获得的知识，并应提供与此主题相关的即将到来的挑战的一瞥。
Since decades, the global community has been facing an environmental crisis, resulting in the need to switch from outdated to new, more efficient energy sources and a more effective way of tackling the rising carbon dioxide emissions. The activation of small molecules such as O2, H+, and CO2 in a cost—and energy-efficient way has become one of the key topics of catalysis research. The main issue concerning the activation of these molecules is the kinetic barrier that has to be overcome in order for the catalyzed reaction to take place. Nature has already provided many pathways in which small molecules are being activated and changed into compounds with higher energy levels. One of the most famous examples would be photosynthesis in which CO2 is transformed into glucose and O2 through sunlight, thus turning solar energy into chemical energy. For these transformations nature mostly uses enzymes that function as catalysts among which porphyrin and porphyrin-like structures can be found. Therefore, the research focus lies on the design of novel porphyrinoid systems (e.g. corroles, porphyrins and phthalocyanines) whose metal complexes can be used for the direct electrocatalytic reduction of CO2 to valuable chemicals like carbon monoxide, formate, methanol, ethanol, methane, ethylene, or acetate. For example the cobalt(III)triphenylphosphine corrole complex has been used as a catalyst for the electroreduction of CO2 to ethanol and methanol. The overall goal and emphasis of this research area is to develop a method for industrial use, raising the question of whether and how to incorporate the catalyst onto supportive materials. Graphene oxide, multi-walled carbon nanotubes, carbon black, and activated carbon, to name a few examples, have become researched options. These materials also have a beneficial effect on the catalysis through for instance preventing rival reactions such as the Hydrogen Evolution Reaction (HER) during CO2 reduction. It is very apparent that the topic of small molecule activation offers many solutions for our current energy as well as environmental crises and is becoming a thoroughly investigated research objective. This review article aims to give an overview over recently gained knowledge and should provide a glimpse into upcoming challenges relating to this subject matter.
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DOI：
10.1073/pnas.1507063112
发表时间：
2015-06-02
影响因子：
11.1
作者：
Costentin, Cyrille;Robert, Marc;Tatin, Arnaud
通讯作者：
Tatin, Arnaud
影响因子：
2.9
作者：
Behar, D;Dhanasekaran, T;Fujita, E
通讯作者：
Fujita, E
影响因子：
56.9
作者：
Costentin, Cyrille;Drouet, Samuel;Saveant, Jean-Michel
通讯作者：
Saveant, Jean-Michel
影响因子：
--
作者：
Bhugun, I;Lexa, D;Saveant, JM
通讯作者：
Saveant, JM
影响因子：
22
作者：
Choi, Jaecheol;Wagner, Pawel;Officer, David L.
通讯作者：
Officer, David L.