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Pt Nanoparticles Supported on Mesoporous Graphitic Carbon Nitride as Catalysts for Hydrolytic Dehydrogenation of Ammonia Borane
ACS Applied Nano Materials ( IF 5.9 ) Pub Date : 2020-06-18 , DOI: 10.1021/acsanm.0c01208
Merve Aksoy 1 , Önder Metin 1, 2, 3
Affiliation  

Platinum (Pt) nanoparticles (NPs) supported on mesoporous graphitic carbon nitride (mpg-CN/Pt) were synthesized in situ via the reduction of as-prepared mpg-CN/Pt(IV) composites during the catalytic hydrolysis of ammonia-borane (AB) under the white-light irradiation. The yielded mpg-CN/Pt nanocatalysts were characterized by using many advanced analytical techniques including TEM, XRD, ICP-MS, XPS, FTIR, PL, and time-resolved emission spectroscopy (TRES) techniques. Besides the privilege advantageous of the presented in situ synthesis protocol for the synthesis of mpg-CN/Pt nanocatalysts, formation of the heterojunction between in situ generated Pt NPs and visible-light active semiconductor mpg-CN enables an improved charge separation and prolonged lifetime, resulting in 2.25-fold enhanced photocatalytic activity within the hydrolysis of AB under white-light irradiation. The effect of Pt loading on the catalytic activity of mpg-CN/Pt nanocatalysts was examined in the hydrolysis of AB and the highest turnover frequency (TOF) of 274.2 min–1 was obtained with 5.94 wt % Pt-loaded mpg-CN/Pt nanocatalysts, which is the one of the best TOFs among monometallic Pt-based nanocatalysts and comparable to the ones reported using bimetallic Pt nanocatalysts. Moreover, mpg-CN/Pt nanocatalysts were found to be highly durable in the hydrolysis of AB such that it preserves 78% of its initial catalytic activity after the 10th consecutive runs, which is one of the highest reusability performances among all Pt-based catalysts that have been tested in the hydrolysis of AB so far. Upon the results of the kinetic studies, the rate law and activation parameters for the mpg-CN/Pt-catalyzed AB hydrolysis were also reported. This work demonstrates for the first time that mpg-CN is a proper support material for the in situ synthesis of catalytically active yet stable Pt NPs promoting the photocatalytic hydrogen evolution from the hydrolysis of AB.

中文翻译:

介孔石墨质氮化碳上负载的Pt纳米颗粒作为氨硼烷水解脱氢的催化剂

在氨硼烷催化水解过程中,通过还原制备的mpg-CN / Pt(IV)复合材料,就地合成了负载在介孔石墨氮化碳(mpg-CN / Pt)上的铂(Pt)纳米颗粒(NPs)。 AB)在白光照射下。通过使用许多先进的分析技术,包括TEM,XRD,ICP-MS,XPS,FTIR,PL和时间分辨发射光谱(TRES)技术,对生成的mpg-CN / Pt纳米催化剂进行了表征。除了所提出的原位合成方案可用于合成mpg-CN / Pt纳米催化剂的特权优势外,在原位生成的Pt NP与可见光活性半导体mpg-CN之间形成异质结还可以改善电荷分离并延长使用寿命,导致2。白光照射下AB水解中的光催化活性提高了25倍。在AB的水解和274.2 min的最高周转频率(TOF)中检查了Pt负载量对mpg-CN / Pt纳米催化剂催化活性的影响。–1用5.94 wt%的Pt载mpg-CN / Pt纳米催化剂制得的Pt纳米催化剂是单金属基于Pt的纳米催化剂中最好的TOF之一,与使用双金属Pt纳米催化剂报道的TOF相当。此外,发现mpg-CN / Pt纳米催化剂在AB的水解中具有很高的耐用性,因此在连续运行10次后仍保留其初始催化活性的78%,这是所有Pt基催化剂中可重复使用性最高的性能之一到目前为止,已经在AB的水解中进行了测试。根据动力学研究的结果,还报道了mpg-CN / Pt催化的AB水解的速率规律和活化参数。
更新日期:2020-07-24
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