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Nb2BN2- cluster anions reduce four carbon dioxide molecules: reactivity enhancement by ligands.
Dalton Transactions ( IF 3.5 ) Pub Date : 2020-09-03 , DOI: 10.1039/d0dt02680h Hai-Yan Zhou 1 , Ming Wang 1 , Yong-Qi Ding 1 , Jia-Bi Ma 1
Dalton Transactions ( IF 3.5 ) Pub Date : 2020-09-03 , DOI: 10.1039/d0dt02680h Hai-Yan Zhou 1 , Ming Wang 1 , Yong-Qi Ding 1 , Jia-Bi Ma 1
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The thermal gas-phase reactions of Nb2BN2− cluster anions with carbon dioxide have been explored by using the art of time-of-flight mass spectrometry and density functional theory calculations. Four CO2 molecules can be consecutively reduced by Nb2BN2−, resulting in the formation of Nb2BN2O1–4− anions and the release of one CO molecule each time. To illustrate the role of ligands in Nb2BN2−, the reactivities of Nb2N2− and Nb2B− toward CO2 were also investigated; two and three CO2 molecules are activated, respectively, and the rate constants are slower than that of Nb2BN2−/CO2 systems. This comparison indicates that metal–metal multiple bonds and appropriate ligands, such as B, are important factors for CO2 reduction. The synergy between a transition metal atom (Nb) and a main-group atom (B) in CO2 reduction mediated by gas-phase clusters is revealed for the first time. To the best of our knowledge, Nb2BN2− anions are gas-phase clusters that reduce the largest number of CO2 molecules. A fundamental understanding of the efficient reduction of carbon dioxide molecules may shed light on the rational design of active sites on supported transition metal/boron nitride catalysts.
中文翻译：
Nb2BN2-团簇阴离子可还原四个二氧化碳分子：配体可提高反应活性。
Nb的热气相反应2 BN 2 -与二氧化碳簇阴离子已通过使用时间飞行质谱和密度泛函理论计算的现有技术的探讨。四CO 2分子可通过Nb的被连续地降低2 BN 2 - ，导致Nb的形成2 BN 2 ö 1-4 -阴离子和每次一个CO分子的释放。为了说明在铌配位体的作用2 BN 2 - ，的铌的反应性2 Ñ 2 -和Nb 2乙-还研究了对CO 2的影响；两个和三个CO 2分子被激活，分别和速率常数比的Nb较慢2 BN 2 - / CO 2的系统。这种比较表明，金属-金属多重键和适当的配体（例如B）是减少CO 2的重要因素。首次揭示了由气相团簇介导的CO 2还原中过渡金属原子（Nb）和主原子（B）之间的协同作用。据我们所知，铌2 BN 2 -阴离子气相簇减少二氧化碳的数量最多2分子。对有效减少二氧化碳分子的基本理解可以为负载型过渡金属/氮化硼催化剂上活性位的合理设计提供启示。
更新日期：2020-10-20
中文翻译：
Nb2BN2-团簇阴离子可还原四个二氧化碳分子：配体可提高反应活性。
Nb的热气相反应2 BN 2 -与二氧化碳簇阴离子已通过使用时间飞行质谱和密度泛函理论计算的现有技术的探讨。四CO 2分子可通过Nb的被连续地降低2 BN 2 - ，导致Nb的形成2 BN 2 ö 1-4 -阴离子和每次一个CO分子的释放。为了说明在铌配位体的作用2 BN 2 - ，的铌的反应性2 Ñ 2 -和Nb 2乙-还研究了对CO 2的影响；两个和三个CO 2分子被激活，分别和速率常数比的Nb较慢2 BN 2 - / CO 2的系统。这种比较表明，金属-金属多重键和适当的配体（例如B）是减少CO 2的重要因素。首次揭示了由气相团簇介导的CO 2还原中过渡金属原子（Nb）和主原子（B）之间的协同作用。据我们所知，铌2 BN 2 -阴离子气相簇减少二氧化碳的数量最多2分子。对有效减少二氧化碳分子的基本理解可以为负载型过渡金属/氮化硼催化剂上活性位的合理设计提供启示。
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