水热法制备Ni/Nd2O3催化剂及其催化水合联氨制氢

doi:10.16085/j.issn.1000-6613.2018-1398

化工进展 ›› 2019, Vol. 38 ›› Issue (05): 2372-2379.DOI: 10.16085/j.issn.1000-6613.2018-1398

水热法制备Ni/Nd₂O₃催化剂及其催化水合联氨制氢

张欢¹(),马敬环¹,马云超²,刘莹¹(),王嘉豪¹,苏彦铭¹,刘晓涯¹,戴莉³

1. 天津工业大学环境与化学工程学院，天津 300387
2. 吉林石化公司工程造价部，吉林吉林 132022
3. 山东农业大学化学与材料科学学院，山东泰安 271018

收稿日期:2018-07-09 修回日期:2018-11-15 出版日期:2019-05-05 发布日期:2019-05-05
通讯作者: 刘莹
作者简介:<named-content content-type="corresp-name">张欢</named-content>（1992—），女，硕士研究生，研究方向为环境催化。E-mail：<email>zhanghuan0716@163.com</email>。
基金资助:
国家自然科学基金(51508384)

Preparation of Ni/Nd₂O₃ catalysts by hydrothermal method and its catalytic decomposition of hydrated hydrazine for hydrogen production

Huan ZHANG¹(),Jinghuan MA¹,Yunchao MA²,Ying LIU¹(),Jiahao WANG¹,Yanming SU¹,Xiaoya LIU¹,Li DAI³

1. School of Environmental and Chemical Engineering, Tianjin Polytechnic University, Tianjin 300387, China
2. Engineering Cost Department of Jilin Petrochemical Company, Jilin 132022, Jilin, China
3. College of Chemistry and Material Science, Shandong Agricultural University, Tai’an 271018, Shandong, China

Received:2018-07-09 Revised:2018-11-15 Online:2019-05-05 Published:2019-05-05
Contact: Ying LIU

摘要/Abstract

摘要：

采用水热合成法制备了Ni/Nd₂O₃催化剂，对其催化水合联氨制氢性能进行了考察，探讨了催化剂合成条件及催化体系中NaOH浓度对催化性能的影响，并采用XRD、XPS、TEM、TG对催化剂进行了分析表征。结果表明，当Ni/Nd=94∶6、水热条件为8h、120℃时，合成的Ni/Nd₂O₃催化剂在催化水合联氨制氢时表现出了最优的催化性能，其H₂选择性为95.9%。该催化剂中Ni的结晶度较高，Nd以Nd₂O₃的形式存在，具有促进颗粒分散、暴露活性位点、协助Ni、Nd电子转移等优点。与不加NaOH溶液的催化制氢体系相比，当NaOH的加入浓度为1.3mol/L时，催化剂催化水合联氨的制氢速率提高了约3.7倍。催化剂可维持良好的稳定性，循环使用5次后H₂选择性仍高达94.4%。

关键词: Ni/Nd₂O₃催化剂, 水热, 合成, 水合联氨, 制氢

Abstract:

Ni/Nd₂O₃ catalyst was prepared by hydrothermal method, and its performance in hydrogen production was investigated. The effects of the catalyst synthesis condition and NaOH concentration on the catalytic performance were discussed, and the catalyst was characterized by XRD, XPS, TEM and TG. The results show that when the catalyst with a Ni/Nd molar ratio of 94∶6 and reaction time 8h at 120℃,the highest H₂ selectivity of 95.9% could be achieved. The crystallinity of Ni of the catalyst is fairly high and the Nd species exist in the form of Nd₂O₃, which is beneficial for promoting particle dispersion, exposing active sites and assisting the electron transfer between Ni and Nd. NaOH with varied concentration can change the alkaline state of the system, compared with the reaction system without NaOH solution. When the NaOH concentration is 1.3mol/L, the hydrogen production rate is increased about 3.7 times. After 5 times of catalyst cycling, the selectivity of H₂ is still up to 94.4%, which indicates that the catalyst by hydrothermal synthesis has good stability.

Key words: Ni/Nd₂O₃ catalyst, hydrothermal, synthesis, hydration hydrazine, hydrogen production

中图分类号:

O643

张欢, 马敬环, 马云超, 刘莹, 王嘉豪, 苏彦铭, 刘晓涯, 戴莉. 水热法制备Ni/Nd₂O₃催化剂及其催化水合联氨制氢[J]. 化工进展, 2019, 38(05): 2372-2379.

Huan ZHANG, Jinghuan MA, Yunchao MA, Ying LIU, Jiahao WANG, Yanming SU, Xiaoya LIU, Li DAI. Preparation of Ni/Nd₂O₃ catalysts by hydrothermal method and its catalytic decomposition of hydrated hydrazine for hydrogen production[J]. Chemical Industry and Engineering Progress, 2019, 38(05): 2372-2379.

图/表 9

图1 不同条件下制备的催化剂的XRD图

表1 不同条件下制备的Ni/Nd=94∶6催化剂晶体的平均粒径

共还

原法

图2 水热法和共还原法合成的Ni/Nd=94∶6催化剂的TEM、HRTEM图

图3 水热法合成的Ni/Nd2O3催化剂和共还原法合成的Ni-Nd2O3 催化剂的XPS谱图

图4 Ni和Ni/Nd2O3催化剂的热重图

图5 不同制备方法下各Ni、Nd比催化剂催化水合联氨产气曲线图

图6 不同水热条件对催化剂催化活性的影响

图7 NaOH浓度对Ni/Nd2O3催化剂催化性能的影响

图8 Ni/Nd2O3催化剂稳定性能测试

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水热法制备Ni/Nd₂O₃催化剂及其催化水合联氨制氢

Preparation of Ni/Nd₂O₃ catalysts by hydrothermal method and its catalytic decomposition of hydrated hydrazine for hydrogen production

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