高温活性位点印迹法制备碳基单原子镍及其二氧化碳还原应用研究  

Preparation of carbon-based single Ni sites by high-temperature active-site imprinting and their application to CO_(2)RR

作　　者：梁心虹 郭宇辰 程风顺 朱远蹠 Liang Xinhong;Guo Yuchen;Cheng fengshun;Zhu Yuanzhi(Yunnan Provincial Key Laboratory of Energy Saving and New Materials in Phosphorus Chemical Engineering,Faculty of Chemical Engineering,Kunming University of Science and Technology,Kunming 650500)

机构地区：[1]昆明理工大学化学工程学院,云南省磷化工节能与新材料重点实验室,昆明650500

出　　处：《化工新型材料》2024年第S02期338-344,共7页New Chemical Materials

基　　金：云南省应用基础研究计划(202101BE070001-032)。

摘　　要：利用具有分级多孔结构且导电性能优异的MOF衍生材料为碳基底,通过设计高温活性位点原子印迹法制备了碳基二氧化碳还原(ECR)催化剂。该方法的优势在于将活性较低的ZnN_(x)或氮空位(V-N_(x))转化为M-N_(x)。通过前驱体(Zn-N-C)合成时加入Super P进行插层,结合高温活性位点印迹制备高活性原子分散的Ni-N-C-sp ECR电催化剂。Super P可对催化剂的局部环境进行协调,并同步提升了碳基底的导电性能。结果表明:碳化后的催化剂具有丰富的孔结构和高活性。Ni-N-C-sp催化剂在-0.76V(vs.RHE)的电位范围内表现出100%的法拉第效率。同时电流密度能够达到33.2mA/cm^(2)。优异的法拉第效率和较大的电流密度表明Ni-N-C-sp催化剂在电催化ECR领域的高适用性。Carbon-based carbon dioxide reduction(ECR)catalysts were prepared by designing high-temperature active site atomic imprinting method using MOF-derived materials with hierarchical pore structure and excellent electrical conductivity as carbon substrates.The advantage of this method was the conversion of less active ZnN_(x)or nitrogen vacancies(V-N_(x))into M-N_(x).Highly active atomically dispersed Ni-N-C-sp ECR electrocatalysts were prepared by the addition of Super P for intercalation during the synthesis of the precursor(Zn-N-C),combined with high-temperature active site imprinting.Super P coordinated the local environment of the catalyst and simultaneously enhanced the conductivity of the carbon substrate.The results showed that the carbonized catalysts had rich pore structure and high activity.Electrochemical tests indicated that the Ni-N-C-sp catalyst exhibited 100%Faraday efficiency in the potential range of-0.76V(vs.RHE).At the same time,the current density was able to reach 33.2mA/cm^(2).The excellent Faraday efficiency and large current density verified the high suitability of the Ni-N-C-sp catalyst for practical electrochemical ECR.

关 键 词：高温活性位点原子印迹法 二氧化碳还原反应 高负载 镍单原子催化剂 

分 类 号：TQ15[化学工程—电化学工业]