当前位置:科学网首页 > 小柯机器人 >详情
金属-有机骨架膜包裹金纳米粒子用于直接等离子体光催化固氮
作者:小柯机器人 发布时间:2021/4/18 14:28:47

北京理工大学王博团队报道了金属-有机骨架膜包裹金纳米粒子用于直接等离子体光催化固氮。 相关研究成果发表在2021年4月13日出版的《美国化学会杂志》。

光催化固氮反应可以获取太阳能,将丰富而惰性的N2转化为NH3。

该文利用金属-有机骨架(MOF)膜作为纳米反应器的理想组装体分散和限制金纳米粒子(AuNPs),实现了环境条件下的直接等离子体光催化固氮。在可见光照射下,金纳米粒子上产生的热电子可以直接注入吸附在金表面的N2分子中。此类N2分子还可以被强而短暂的局部表面等离子体共振场激活,从而使氨的析出速率具有超线性的强度依赖性,在强辐照下具有更高的表观量子效率和更低的表观活化能。

此外,由多个相互连接的纳米反应器组成的可渗透的Au @ MOF膜可以确保AuNP的分散性和稳定性,进一步促进N2分子和(水合的)质子的质量转移,并在设计的气体中促进等离子体的光催化反应。结果表明,在可见光下(>400nm,100mW cm-2)氨的析出速率为18.9mmol-gAu-1h-1,在520nm处的表观量子效率为1.54%。

附:英文原文

Title: Metal–Organic Framework Membranes Encapsulating Gold Nanoparticles for Direct Plasmonic Photocatalytic Nitrogen Fixation

Author: Li-Wei Chen, Yu-Chen Hao, Yu Guo, Qinghua Zhang, Jiani Li, Wen-Yan Gao, Lantian Ren, Xin Su, Linyu Hu, Nan Zhang, Siwu Li, Xiao Feng, Lin Gu, Ya-Wen Zhang, An-Xiang Yin, Bo Wang

Issue&Volume: April 13, 2021

Abstract: Photocatalytic nitrogen fixation reaction can harvest the solar energy to convert the abundant but inert N2 into NH3. Here, utilizing metal–organic framework (MOF) membranes as the ideal assembly of nanoreactors to disperse and confine gold nanoparticles (AuNPs), we realize the direct plasmonic photocatalytic nitrogen fixation under ambient conditions. Upon visible irradiation, the hot electrons generated on the AuNPs can be directly injected into the N2 molecules adsorbed on Au surfaces. Such N2 molecules can be additionally activated by the strong but evanescently localized surface plasmon resonance field, resulting in a supralinear intensity dependence of the ammonia evolution rate with much higher apparent quantum efficiency and lower apparent activation energy under stronger irradiation. Moreover, the gas-permeable Au@MOF membranes, consisting of numerous interconnected nanoreactors, can ensure the dispersity and stability of AuNPs, further facilitate the mass transfer of N2 molecules and (hydrated) protons, and boost the plasmonic photocatalytic reactions at the designed gas–membrane–solution interface. As a result, an ammonia evolution rate of 18.9 mmol gAu–1 h–1 was achieved under visible light (>400 nm, 100 mW cm–2) with an apparent quantum efficiency of 1.54% at 520 nm.

DOI: 10.1021/jacs.0c13342

Source: https://pubs.acs.org/doi/10.1021/jacs.0c13342

 

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000