脱合金效应提升NiRu@C催化剂的析氢性能  

De-Alloyed NiRu@C Catalyst With Enhanced Electrocatalytic Performance for Hydrogen Evolution Reaction

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作  者:袁迎 郑路凡 荣峻峰 YUAN Ying;ZHENG Lufan;RONG Junfeng(SINOPEC Research Institute of Petroleum Processing Co.,Ltd.,Beijing 100083,China)

机构地区:[1]中石化石油化工科学研究院有限公司,北京100083

出  处:《石油学报(石油加工)》2023年第6期1251-1262,共12页Acta Petrolei Sinica(Petroleum Processing Section)

基  金:国家自然基金重点项目(U21B2092)资助。

摘  要:电催化析氢反应(HER)是获得可再生氢能的有效策略,但电催化析氢催化剂活性和稳定性仍有待提高。基于此,通过热解镍盐、钌盐、柠檬酸的络合物制备了碳包覆镍钌催化剂,为了克服该催化剂中Ru原子利用率低的缺点,采用乙酸对碳包覆镍钌催化剂进行刻蚀制备脱合金NiRu@C催化剂。通过XRD、BET、ICP等手段对脱合金NiRu@C催化剂进行表征,在摩尔浓度1.0 mol/L KOH电解质中测定脱合金NiRu@C催化剂的电催化析氢性能。结果表明:脱合金处理后,Ni从NiRu晶格中溶解出来,形成富Ru的多孔结构,Ni的溶出造成催化剂结构及晶格参数的改变,多孔结构的形成使催化剂比表面积大幅度增加,增加了Ru活性位点的暴露;脱合金NiRu@C催化剂具有优异的HER活性,在电流密度10 mA/cm^(2)下过电位仅为36 mV,与未脱合金的NiRu@C催化剂相比,HER性能提升4倍,优于商业Pt/C催化剂(40 mV)。脱合金策略为优化HER活性提供一种新的思路。Electrocatalytic hydrogen evolution reaction(HER)is an effective strategy to obtain renewable hydrogen energy.However,the activity and stability of electrocatalytic hydrogen evolution catalyst still need to be improved.Based on this,carbon coated nickel ruthenium catalysts were prepared by pyrolyzing the complexes of nickel salt,ruthenium salt and citric acid.To avoid the low utilization rate of Ru atom in this catalyst,the carbon-coated NiRu catalysts were etched by acetic acid to prepare de-alloyed NiRu@C catalysts.The de-alloyed NiRu@C catalysts were characterized by XRD,BET,and ICP.The electrocatalytic hydrogen evolution performance of de-alloyed NiRu@C catalysts was determined in 1.0 mol/L KOH electrolyte.The results show that the Ni dissolved out of the NiRu lattice after the de-alloying treatment to form the Ru-rich porous structure.The dissolution of Ni caused changes in the catalyst structure and lattice parameters,and the formation of porous structure led to an increase in the catalyst specific surface area and the exposure of Ru active sites.The de-alloyed NiRu@C catalyst exhibited excellent HER activity with an overpotential of only 36 mV at the current density of 10 mA/cm^(2),and has a 4-fold improvement in HER performance as compared with un-alloyed NiRu@C catalyst,which is better than commercial Pt/C catalyst(40 mV).The de-alloying strategy provides a new strategy for optimizing HER activity.

关 键 词:电催化析氢 碳包覆 镍钌催化剂 脱合金 过电位 电流密度 构效关系 

分 类 号:TQ151[化学工程—电化学工业]

 

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