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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >The good, the neutral, and the positive: buffer identity impacts CO2 reduction activity by nickel(ii) cyclam
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The good, the neutral, and the positive: buffer identity impacts CO2 reduction activity by nickel(ii) cyclam

机译：良好的，中性和阳性：缓冲率标识会影响镍（II）锡的二氧化碳减少活性

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摘要

Development of new synthetic catalysts for CO2 reduction has been a central focus of chemical research efforts towards mitigating rising global carbon dioxide levels. In parallel with generating new molecular systems, characterization and benchmarking of these compounds across well-defined catalytic conditions are essential. Nickel(ii) cyclam is known to be an active catalyst for CO2 reduction to CO. The degree of selectivity and activity has been found to differ widely across electrodes used and upon modification of the ligand environment, though without a molecular-level understanding of this variation. Moreover, while proton transfer is key for catalytic activity, the effects of varying the nature of the proton donor remain unclear. In this work, a systematic investigation of the electrochemical and light-driven catalytic behaviour of nickel(ii) cyclam under different aqueous reaction conditions has been performed. The activity and selectivity are seen to vary widely depending on the nature of the buffering agent, even at a constant pH, highlighting the importance of proton transfer for catalysis. Buffer binding to the nickel center is negatively correlated with selectivity, and cationic buffers show high levels of selectivity and activity. These results are discussed in the context of molecular design principles for developing increasingly efficient and selective catalysts. Moreover, identifying these key contributors towards activity has implications for understanding the role of the conserved secondary coordination environments in naturally occurring CO2-reducing enzymes, including carbon monoxide dehydrogenase and formate dehydrogenase.
机译：CO2减少新的合成催化剂的开发是化学研究努力减轻了全球二氧化碳水平上升的核心焦点。与产生新的分子系统并行，在良好定义的催化条件下这些化合物的表征和基准是必要的。已知镍（II）循环氨酸是CO 2的活性催化剂，用于CO。已经发现选择性和活性的程度在使用的电极和改性配体环境时不同，但没有分子水平的理解变化。此外，虽然质子转移是催化活性的关键，但是改变质子供体的性质的影响仍然不清楚。在这项工作中，已经进行了在不同水性反应条件下进行了对镍（II）圈的电化学和光驱动催化行为的系统研究。认为活动和选择性根据缓冲剂的性质，即使在恒定的pH下也突出了质子转移对催化的重要性。与镍中心结合的缓冲液与选择性呈负相关，阳离子缓冲液显示出高水平的选择性和活性。这些结果在分子设计原理的上下文中讨论了越来越有效和选择性催化剂。此外，鉴定对活动的这些关键贡献者对理解保守的二级配合环境在天然存在的二氧化碳酶中的作用具有影响，包括一氧化碳脱氢酶和甲酯脱氢酶。

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