可见光引发石墨烯发射电子促进的常压下氨合成
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- 英文论文题名：Atmospheric Ammonia Synthesis Promoted by Hot Electrons from Graphene Induced by Visible Light
- 论文作者：卢艳红 ; 杨扬 ; 张腾飞 ; 陈永胜
- 英文论文作者：Yanhong Lu ; Yang Yang ; Tengfei Zhang ; Yongsheng Chen ; School of Chemistry & Material Science ; Langfang Teachers University ; College of Chemistry ; Nankai University
- 年：2016
- 作者机构：廊坊师范学院;南开大学;
- 论文关键词：三维石墨烯 ; 发射电子 ; 光催化 ; 氨合成
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十九分会：纳米碳材料
- 语种：中文
- 分类号：O643.36;TQ113.21
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十九分会 ; 纳米碳材料
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：221k
- 原文格式：D
- 会议级别：全国
摘要
本文以氧化石墨烯和硝酸铁为原料,采用溶剂热方法制备了三维石墨烯负载纳米氧化铁的复合材料。通过X-射线衍射光谱、拉曼光谱、扫描电镜、透射电镜、X-射线光电光谱及等离子体原子发射光谱等方法对材料的结构和性能进行了表征。利用在光照下三维石墨烯可以发射出热(自由)电子的性质,以此复合材料作为光催化剂,在常压下实现了氨的合成。实验表明,在紫外、可见及红外光宽波谱范围下,三维石墨烯发射出的热(自由)电子可以有效地促进合成氨原料气N_2和H_2的裂解,从而实现在不需要高温、高压以及电化学辅助,在常压光照的温和条件下氨的合成。并且,氨的合成速率与激发光的频率(同强度)和强度(同频率)成良好的线性关系。通过对中间体和活化能的检测,对此合成氨的活化机理和反应历程进行了阐述。同时,对催化剂的光催化稳定性进行了研究,通过结构助剂的加入,催化剂的活性可以保持在50小时以上。
Here we demonstrate that using an iron and graphene based catalyst, Fe@3DGraphene, hot(ejected) electrons from this composite catalyst induced by visible light in wide range of wavelength up to red, could efficiently facilitate the activation of N_2 and generate ammonia with H_2 directly at atmospheric pressure using light(including simulated sun light) illumination directly. No external voltage or electrochemical or any other agent is needed. The production rate increases with increasing light frequency under the same power and with increasing power under the same frequency. The mechanism is confirmed by the detection of the intermediate N_2H_4 and also with a measured apparent activation energy only ~1/4 of the iron based Haber-Bosch catalyst. Combined with a morphology control using alumina as the structural promoter, the catalyst retains its activity in a 50-hour test.
Here we demonstrate that using an iron and graphene based catalyst, Fe@3DGraphene, hot(ejected) electrons from this composite catalyst induced by visible light in wide range of wavelength up to red, could efficiently facilitate the activation of N_2 and generate ammonia with H_2 directly at atmospheric pressure using light(including simulated sun light) illumination directly. No external voltage or electrochemical or any other agent is needed. The production rate increases with increasing light frequency under the same power and with increasing power under the same frequency. The mechanism is confirmed by the detection of the intermediate N_2H_4 and also with a measured apparent activation energy only ~1/4 of the iron based Haber-Bosch catalyst. Combined with a morphology control using alumina as the structural promoter, the catalyst retains its activity in a 50-hour test.
引文
[1]Zhang,T.;Chang,H.;Wu,Y.;Xiao,P;Yi,N et al.Nat.Photon.2015,9:471.
[2]Wu,Y.;Yi,N.;Huang,L.;Zhang,T.;Fang,S.et al.Nat.Commun.2015,6:6141.
[2]Wu,Y.;Yi,N.;Huang,L.;Zhang,T.;Fang,S.et al.Nat.Commun.2015,6:6141.