论文标题
单原子锚定的新型二维MOSI2N4单层，可有效地将CO2电化为甲酸和甲烷
Single-atom anchored novel two-dimensional MoSi2N4 monolayers for efficient electroreduction of CO2 to formic acid and methane
论文作者
论文摘要
有效，有选择性的二氧化碳将作为二氧化碳转化率的重要方法出现到增值化学物质和燃料中，但是，它依赖于具有可控的产品选择性和反应路径的催化剂。在这项工作中，通过第一原理计算，我们确定了五个催化剂（TM@Mosi2N4，TM = SC，Ti，Fe，Fe，Co和Ni），其中包括固定在MOSI2N4单层上的过渡金属原子，该原子的催化性能可以通过调节D-Band中心和支持的金属占用的催化性能来控制其催化性能。在二氧化碳还原过程中，单个金属原子作为活性位点功能激活MOSI2N4惰性基础平面，而AS设计的电催化剂在CO2还原方面具有出色的活性。有趣的是，HCOOH是CO@MOSI2N4催化剂上二氧化碳减少的首选产品，其速率确定为0.89 eV，而其他四个催化剂则希望以0.81-1.24 ev的速率确定性屏障将CO2降低至CH4。此外，MOSI2N4是一种极为空气的材料，它将促进其在各种环境中的应用。我们的发现提供了一个有希望的候选人，具有较高的活性，可再生能源技术的催化剂以及实验工作的选择性。
Efficient and selective CO2 electroreduction into value-added chemicals and fuels emerged as a significant approach for CO2 conversion, however, it relies on catalysts with controllable product selectivity and reaction paths. In this work, by means of first-principles calculations, we identify five catalysts (TM@MoSi2N4, TM = Sc, Ti, Fe, Co and Ni) comprising transition-metal atoms anchored on a MoSi2N4 monolayer, whose catalytic performance can be controlled by adjusting the d-band center and occupation of supported metal atoms. During CO2 reduction, the single metal atoms function as the active sites activates the MoSi2N4 inert basal-plane, and as-designed electrocatalysts exhibit excellent activity in CO2 reduction. Interestingly, HCOOH is the preferred product of CO2 reduction on the Co@MoSi2N4 catalyst with a rate-determining barrier of 0.89 eV, while the other four catalysts prefer to reduce CO2 to CH4 with a rate-determining barrier of 0.81-1.24 eV. Moreover, MoSi2N4 is an extremely-air-stable material, which will facilitate its application in various environments. Our findings provide a promising candidate with high activity, catalysts for renewable energy technologies, and selectivity for experimental work.
