高选择性还原二氧化碳制合成气的铜基低成本双金属催化剂的设计与性能测试

Increasing anthropogenic CO2 emission is forecasted to have potentially disastrous effects on global warming and ocean acidification, which becomes an important challenge for the society. The catalytic reduction of CO2 for syngas, will not only effectively reduce CO2 emission, but also produce valuable raw materials for Fischer–Tropsch process in industry. In order to overcome the problem that the most frequently used catalysts for the highly selective reduction of CO2 to produce syngas are with high cost, limited resource storage, and low stability, this proposal is conducted to design Cu-based low-cost bimetallic catalysts with high activity, high selectivity and good stability for the reduction of CO2 for syngas. In this proposal, based on density functional theory (DFT), we will adjust the composition of Cu-based bimetallic catalysts, optimize the binding energies of important reaction intermediates carboxyl group (*HOCO) and activated-carbon monoxide (*CO) with catalytic surfaces, enhance the selectivity of Cu-based low-cost bimetallic catalysts for syngas production pathway, so as to design new Cu-based low-cost bimetallic catalysts with high activity, high selectivity and good stability for the reduction of CO2 for syngas. The project proposed here applies DFT calculations to design catalyst for selective CO2 reduction, helps to extensively reduce the experimental time and cost, and provides useful insight for future large-scale CO2 utilization.

CO2的大量排放，将使全球气候变暖和海洋酸化，成为当今社会发展面临的重大挑战。CO2催化还原制合成气，不仅能有效减少CO2的排放，还能产生化工中费托反应的原料。为克服目前应用于高选择性还原CO2制合成气的催化剂存在成本高、资源有限和易失活等问题，本项目旨在设计具有高活性、高选择性和高稳定性的应用于CO2还原制合成气的铜基低成本双金属催化剂。本项目提出基于密度泛函理论(DFT)，通过调控Cu基双金属催化剂的组成，优化CO2还原制合成气的重要中间基团羧基(*HOCO)和活性一氧化碳基团(*CO)在催化剂表面的结合能，提高Cu基低成本双金属催化剂对生成合成气路径的选择性，从而设计应用于CO2制合成气的高活性、高选择性和高稳定性的新型低成本双金属催化剂的思路。本项目用DFT计算设计用于高选择性还原二氧化碳的催化剂，节约了大量的实验时间与成本，为未来大规模的二氧化碳资源化利用提供了有利导向。

CO2的大量排放，将使全球气候变暖和海洋酸化，成为当今社会发展面临的重大挑战。CO2的催化还原，不仅能有效减少CO2的排放，还能生成价值更高的各类化工原料。当前研究的热点之一提高CO2催化还原的产物选择性，它能有效降低后续的分离成本。同时，为克服目前应用于高选择性还原CO2的催化剂存在成本高、资源有限和易失活等问题，本项目旨在设计具有高活性、高选择性和高稳定性的应用于CO2催化还原的低成本催化剂。本项目提出基于密度泛函理论(DFT)，通过调控催化剂的组成与结构，优化CO2还原反应过程中的重要中间基团羧基(*HOCO)和活性一氧化碳基团(*CO)在催化剂表面的结合能，提高催化剂对反应路径的选择性，从而设计应用于CO2还原的高活性、高选择性和高稳定性的新型低成本催化剂的思路。本项目采用DFT计算与实验测试相结合的方式来设计用于高选择性还原二氧化碳的催化剂，为未来大规模的二氧化碳资源化利用提供了有利导向。