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中空多孔碳球对铂纳米颗粒的限制:在析氢反应中通过孔调节提高活性和耐久性。

Confinement of Pt NPs by hollow-porous-carbon-spheres pore regulation with promoted activity and durability in the hydrogen evolution reaction.

作者信息

Gan Zhuofan, Shu Chengyong, Deng Chengwei, Du Wei, Huang Bo, Tang Wei

机构信息

School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, P. R. China.

State Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power Sources, Shanghai, 200245, P. R. China.

出版信息

Nanoscale. 2021 Nov 11;13(43):18273-18280. doi: 10.1039/d1nr04982h.

Abstract

Electrochemical water splitting is a promising method to generate pollution-free and sustainable hydrogen energy. However, the specific activity and durability of noble metal catalysts is the main hindrance to the hydrogen evolution reaction. Based on the continuous pore regulation of hollow porous carbon spheres (N-HPCSs) by hexadecyl trimethyl ammonium bromide, the 6.21 wt% Pt/N-HPCSs exhibited good dispersibility, according to a low overpotential of 45 mV (10 mA cm/1 M KOH). Its mass activity was 4 times that of the commercial 20 wt% Pt/C at -0.07 V ( RHE) potential. We analyse that the excellent activity is due to the interaction between Pt nanoparticles and N-HPCSs so that the electron density around the Pt atoms increases, which is beneficial for HO to obtain electrons and transform into H. Meanwhile the sea urchin-like structure of N-HPCSs facilitates the desorption of H. Furthermore, the overpotential showed no obvious decrease in the long-term durability test, which should be attributed to the confinement of Pt nanoparticles by the well-defined pores in N-HPCSs to avoid the aggregation of Pt nanoparticles during long-term testing.

摘要

电化学水分解是一种很有前景的产生无污染且可持续氢能的方法。然而,贵金属催化剂的比活性和耐久性是析氢反应的主要障碍。基于十六烷基三甲基溴化铵对中空多孔碳球(N-HPCSs)进行的连续孔调控,6.21 wt%的Pt/N-HPCSs表现出良好的分散性,在1 M KOH中,其过电位低至45 mV(10 mA cm)。在-0.07 V(RHE)电位下,其质量活性是商业20 wt% Pt/C的4倍。我们分析认为,优异的活性归因于Pt纳米颗粒与N-HPCSs之间的相互作用,使得Pt原子周围的电子密度增加,这有利于HO获得电子并转化为H。同时,N-HPCSs的海胆状结构促进了H的解吸。此外,在长期耐久性测试中过电位没有明显下降,这应归因于N-HPCSs中明确的孔对Pt纳米颗粒的限制,从而避免了长期测试过程中Pt纳米颗粒的聚集。

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