【摘要】 为了改善粉末状电催化剂在高电流密度下运行析氢反应时的催化位点堵塞、活性位点暴露率下降和活性层易剥落等问题，通过真空抽滤方法制备了一种亲水的、具有一定机械柔性的Ti₃C₂T_x/碳化聚丙烯腈纳米纤维（Ti₃C₂T_x/CPAN）自支撑电极。通过改变Ti₃C₂T_x纳米片和碳纳米纤维的比例，得到最优性能的Ti₃C₂T_x/CPAN-2自支撑电极，其在电流密度为50 mA/cm²时的过电位为514 mV,Tafel斜率为187 mV dec^-1。进一步利用Ti₃C₂T_x纳米片表面终端基团的还原性，在Ti₃C₂T_x/CPAN-2上原位还原Pd纳米粒子，得到Ti₃C₂T_x/CPAN-2@Pd自支撑电极。得益于Ti₃C₂T_x与原位生成的Pd之间的金属-载体相互作用，增加了载体界面和金属的结合强度，Ti₃C₂T_x/CPAN-2@Pd在电流密度为50 mA/cm²时的过电位为181 mV,Tafel斜率为130 mV dec^-1，且比商用Pd/C具有更佳的CV循环稳定性，体现了其在高电流密度下运行稳定的析氢反应的潜力。更多还原

【Abstract】 To address issues such as catalytic site blockage, decreased exposure rate of active sites, and easy delamination of active layers in powdered electrocatalysts during the hydrogen evolution reaction（HER）under high current densities, a hydrophilic and mechanically flexible self-supporting Ti₃C₂T_x/carbonized polyacrylonitrile nanofiber（Ti₃C₂T_x/CPAN） electrode was prepared via a simple vacuum filtration method. By adjusting the ratio of Ti₃C₂T_xnanosheets to carbon nanofibers, the optimal Ti₃C₂T_x/CPAN-2 self-supporting electrode was obtained, exhibiting an overpotential of 514 mV and a Tafel slope of 238 mV dec^-1at a current density of 50 mA cm^-2. Furthermore, leveraging the reducibility of terminal groups on the surface of Ti₃C₂T_x nanosheets, Pd was in situ reduced on Ti₃C₂T_x/CPAN-2 to fabricate a Ti₃C₂T_x/CPAN-2@Pd self-supporting electrode. Benefiting from the metal-support interaction between Ti₃C₂T_xand in situ-generated Pd, which enhanced the inter-facial bonding strength between the support and the metal, the Ti₃C₂T_x/CPAN-2@Pd electrode demonstrated an improved over-potential of 181 mV and a Tafel slope of 130 mV dec^-1at 50 mA cm^-2.Additionally, it exhibited superior cyclic voltammetry（CV） stability compared to commercial Pd-C, confirming its feasibility for stable HER operation under high current densities.更多还原