摘要：The conversion of inert N_(2) and CO_(2) into urea by electrocatalytic technology not only reduces the cost of urea synthesis in future,but also alleviatesthe environmental pollution problem caused by carbon emission in traditional industrial ***,facing downside factors such as strong competitive reactions and unclear reaction mechanism,the design of high-performance urea catalysts is *** study demonstrates that W_(18)O_(49) system doped heteronuclear metals(TM=Fe,Co,Ni)can effectively solve the problem of competitive adsorption between N_(2) and CO_(2) and realize the co-adsorption of N_(2) and CO_(2) at diverse *** theoretical limiting voltages for urea production on TM-W_(18)O_(49)(TM=Fe,Co,Ni)systems are-0.46 V,-0.42 V and-0.52 V,*** results are all lower than that of the contrastive voltage in pristine W_(18)O_(49) system(-0.91 V),further indicating the rationality and necessity of single-atom doped strategy for the co-reduction of two ***,Co-W_(18)O_(49) can theoretically inhibit the side reactions of NRR,CO_(2)RR,and HER,which deserve future experimental exploration in *** study suggests that doping heteronuclear metal into transition metal oxides is a feasible scheme to solve competitive adsorption and improve catalytic performance.

摘要：由可见光驱动的将CO_(2)转化为高附加值燃料是一种清洁可再生的技术,有助于控制全球变暖和应对能源短缺.近年来,二维的金属偶氮盐框架(2D MAFs)因其特定的电子传输路径、高度暴露的表面活性位点及可调节的吸光能力,在CO_(2)光还原研究中备受关注.然而,对其在该领域的研究仍处于初级阶段.本文设计了一种新型二维MAFs(compound 1),通过四-(4-四唑基苯基)乙烯(H;4;TTPE)与钴的自组装实现了对CO_(2)的光还原.作为对比,通过类似的合成过程构建了具有三维结构的compound 2.非均相光催化实验结果显示,2D compound 1的光还原性能明显优于3D compound 2,在相同条件下,其CO产率高达11.56 mmol g^(-1)h^(-1),是compound 2(1.94 mmol g^(-1)h^(-1))的6倍.这一性能优势源于compound 1独特的二维结构,其不仅具有有利于CO_(2)还原的能级,还能在整个CO_(2)光还原过程中促进电子-空穴高效分离.本工作为设计适用于高效CO_(2)光还原的2D MAFs光催化剂指引了方向.