AuPt alloy nanoparticles supported on graphitic carbon nitride: In situ synthesis and superb catalytic performance in the light-assisted hydrolytic dehydrogenation of ammonia borane

AuPt alloy nanoparticles supported on graphitic carbon nitride: In situ synthesis and superb catalytic performance in the light-assisted hydrolytic dehydrogenation of ammonia borane
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DOI:
10.1016/j.apsusc.2022.154286
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发表时间:
2022-07-21
影响因子:
6.7
通讯作者:
Metin, Onder
Metin, Onder
中科院分区:
材料科学1区
文献类型:
--
作者:
Aksoy, Merve;Korkut, Sibel Eken;Metin, Onder

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通过原位合成以石墨氮化碳(GCN)为载体的双金属Au-Pt合金纳米颗粒(NPs),提高了铂基纳米催化剂在氨水解硼烷(AB)反应中的催化活性。所提出的原位合成方法制备的GCN/AuxPt100-x(x=0,8,15,33)纳米催化剂具有高度分散的AuxPt100-x纳米粒子,其平均粒径在GCN纳米片上的变化范围为1.6-2.6 nm。在白光照射下,纳米催化剂GCN/Pt92Au8(600.3 molH-2molPt-(1)min(-1))和GCN/Pt85Au15(587.1 molH2 molPt-1min(-1))的催化活性高于GCN/Pt100(525.7 molH-2molPt-1min(-1)),这是由于Au-Pn和Gcn之间形成的异质结所引起的协同效应。对GCN/AuxPt100-x纳米催化剂的光物理性质进行了详细的表征,结果表明,GCN/AuxPt100-x纳米催化剂的催化活性的提高归功于电荷动力学的改善、更高的光吸收以及从GCN到双金属AuPT合金NPs的有效电子转移通道。通过清除剂研究,阐明了光生载体在光催化AB脱氢反应中的作用。这项研究表明,在AB的常温水解过程中,可以原位制备GCN/AuxPt100-x纳米催化剂,所得到的纳米催化剂对AB的光助水解产氢有显著的促进作用。
Addressed herein is the enhancement of catalytic activity of Pt-based nanocatalysts in the hydrolysis of ammonia borane (AB) via in-situ synthesis of bimetallic AuPt alloy nanoparticles (NPs) supported on graphitic carbon nitride (gCN). The presented in-situ synthesis protocol yielded gCN/AuxPt100-x (x = 0, 8, 15, 33) nanocatalysts with highly dispersed AuxPt100-x NPs having the average particle sizes varied in the range of 1.6-2.6 nm over the gCN nanosheets. The generated gCN/Pt92Au8 (600.3 mol H-2 mol Pt-(1) min(-1)) and gCN/Pt85Au15 (587.1 mol H2 mol Pt-1 min(-1)) nanocatalysts showed higher catalytic activity compared to gCN/Pt-100 (525.7 mol H-2 mol Pt-1 min(-1)) under white-light irradiation, attributed to the synergistic effects aroused in the AuPt alloy NPs and heterojunctions formed between gCN and AuPt alloy NPs. The detailed characterization of photophysical properties of gCN/AuxPt100-x nanocatalysts revealed that their boosted catalytic activity is attributed to the improved charge kinetics, higher light absorption, and effective electron transfer channels from gCN to the bimetallic AuPt alloy NPs. The role of photogenerated carriers in the photocatalytic AB dehydrogenation was also elucidated via scavenger studies. This study shows that gCN/AuxPt100-x nanocatalysts can be prepared in situ during the hydrolysis of AB at room temperature and the yielded nanocatalysts have a significant role in boosting the hydrogen production from the light-assisted hydrolysis of AB.