Department of Chemistry, University of Gour Banga, Malda - 732103, India.
Phys Chem Chem Phys. 2019 Apr 3;21(14):7483-7490. doi: 10.1039/c9cp00133f.
Gas phase hydrogenation of CO2 to HCO2- by coinage-metal hydride anions, MH- (M = Cu, Ag and Au), has been studied with the help of high level computational methodologies. We demonstrate that these hydride anions perform excellently in the specific hydrogenation of CO2 to HCO2-. More precisely, AgH- is shown to be very active for this particular purpose. We show that CO2 activation through the M-HCO2 pathway passes through a very low energy barrier and produces HCO2-; even the metal centered activation (H-MCO2) also leads to the same product through an energy barrier less than 15 kcal mol-1. A closer inspection demonstrates that electronegativity, size of the metal and hydricity of the MH- species control the overall hydrogenation process.
利用高级计算方法研究了金属氢化物阴离子 MH-（M = Cu、Ag 和 Au）将 CO2 气相氢化生成 HCO2-。我们证明了这些氢化物阴离子在 CO2 氢化生成 HCO2-的特定反应中表现出色。更准确地说，AgH-被证明对此具有很高的活性。我们表明，通过 M-HCO2 途径的 CO2 活化需要通过非常低的能垒，生成 HCO2-；即使是金属中心活化（H-MCO2）也能通过小于 15 kcal mol-1 的能垒生成相同的产物。进一步的研究表明，电负性、金属尺寸和 MH-物种的氢化物亲合力控制着整个氢化过程。
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