稻壳基碳材料负载钌催化剂的制备及其对氨硼烷水解制氢的催化性能

吴慧; 郑君宁; 左佑华; 许立信; 叶明富; 万超

doi:10.1016/S1872-5813(23)60349-4

稻壳基碳材料负载钌催化剂的制备及其对氨硼烷水解制氢的催化性能

doi: 10.1016/S1872-5813(23)60349-4

吴慧¹,
郑君宁¹,
左佑华¹,
许立信^1, ,,
叶明富^{1, 2, 3},
万超^{1, 2, 4, 5, ,}

1.
安徽工业大学化学与化工学院, 安徽马鞍山 243000
2.
南开大学先进能源材料化学教育部重点实验室, 天津 300071
3.
宁德师范学院绿色能源与环境催化福建高校重点实验室, 福建宁德 352100
4.
浙江大学化学工程与生物工程学院, 浙江杭州 310027
5.
常州大学江苏省绿色催化材料与技术重点实验室, 江苏常州 213164

基金项目: 国家自然科学基金青年基金(22108238) 和联合项目(U22A20408)，安徽省自然科学基金青年基金(1908085QB68)，中国博士后面上项目(2019M662060)、派出项目(PC2022046)和特别资助站中项目(2020T130580)，江苏省绿色催化材料与技术重点实验室(BM2012110)和绿色能源与环境催化福建省高校重点实验室开放课题(FJ-GEEC202204)和2022年国家级大学生创新创业训练计划项目(202210360037)资助

详细信息

通讯作者:
E-mail: lxxu@hotmail.com

wanchao@zju.edu.cn

中图分类号: O643.36
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- 被引次数: 0
出版历程
- 收稿日期: 2023-01-09
- 修回日期: 2023-02-26
- 录用日期: 2023-03-10
- 网络出版日期: 2023-03-14
- 刊出日期: 2023-08-01

Preparation of rice husk-based carbon supported ruthenium catalyst for the hydrolysis of ammonia borane to produce hydrogen

WU Hui¹,
ZHENG Jun-ning¹,
ZUO You-hua¹,
XU Li-xin^{1
, ,},
YE Ming-fu^{1, 2, 3},
WAN Chao^{1, 2, 4, 5
, ,}

1.
School of Chemistry and Chemical Engineering, Anhui University of Technology, Anhui Ma’anshan 243000, China
2.
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin 300071, China
3.
Key Laboratory of Green Energy and Environment Catalysis (Ningde Normal University), Fujian Province University, Ningde 352100, China
4.
College of Chemical Engineering and Biological Engineering, Zhejiang University, Hangzhou 310027, China
5.
Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Changzhou University, Changzhou 213164, China

Funds: The project was supported by the National Natural Science Foundation of China (22108238, U22A20408), Anhui Provincial Natural Science Foundation (1908085QB68), China Postdoctoral Science Foundation (2019M662060, PC2022046, 2020T130580), Open Research Funds of Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology (BM2012110), Open Research Funds of Key Laboratory of Green Energy and Environment Catalysis (FJ-GEEC202204) and 2022 National Undergraduate Innovation and entrepreneurship training program (202210360037)

摘要

摘要: 本研究采用简单的浸渍还原法，在N₂气氛下高温焙烧三聚氰胺和稻壳来制备氮掺杂稻壳活性炭载体(N-RHC)，再采用RuCl₃溶液通过浸渍法将活性组分Ru负载到N-RHC载体上，得到Ru/N-RHC催化剂，探究了其对氨硼烷制氢的催化性能。结果表明，Ru负载量为5%（质量分数）的Ru/N-RHC催化剂具有较好的氨硼烷制氢催化性能，反应转化频率（TOF）达83.71 min⁻¹，在光的照射下，该催化剂上氨硼烷水解的活化能从88.9 kJ/mol降到64.9 kJ/mol，且制氢速率与氨硼烷浓度以及催化剂浓度呈现正相关。
- 钌催化剂 /
- 氨硼烷 /
- 水解制氢 /
- 生物质炭材料
Abstract: An efficient dehydrogenation catalyst is crucial for the application of ammonia borane (NH₃BH₃, AB) as a solid chemical hydrogen storage material. In this work, a kind of nitrogen-doped rice husk activated carbon (N-RHC) was prepared by roasting melamine and rice husk at high temperature under nitrogen atmosphere. With N-RHC as the support, the rice husk-based carbon supported ruthenium catalyst (Ru/N-RHC) was prepared through impregnation with the RuCl₃ solution and its catalytic performance in the hydrolysis of ammonia borane to produce hydrogen was investigated. The results indicate that the Ru/N-RHC catalyst with a Ru loading of 5% performs excellently in the hydrolysis of ammonia borane; the reaction turnover frequency (TOF) reaches 83.71 min⁻¹ and the apparent activation energy decreases from 88.9 to 64.9 kJ/mol under light irradiation. In addition, the hydrogen production rate is positively correlated with the content of ammonia borane and catalyst.
- ruthenium catalyst /
- ammonia borane /
- hydrogen production by hydrolysis /
- biochar material

HTML全文

FIG. 2586. FIG. 2586.

FIG. 2586. FIG. 2586.

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图 1 ((a)、(b)) 5%Ru/N-RHC_{0.5-873 K} 催化剂不同放大倍数下的TEM 照片; (c) 5%Ru/N-RHC_{0.5-873 K} 催化剂的HAADF照片; (d) C, (e) N, (f) Ru 三种元素的分布

Figure 1 ((a), (b)) TEM images of 5%Ru/N-RHC_{0.5-873 K} with different magnification; (c) HADDF images and elemental mapping of C (d), N (e) and Ru (f) elements for the 5%Ru/N-RHC_{0.5-873 K} catalysts

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图 2 (a) 5%Ru/N-RHC_{0.5-873 K}催化剂的XRD谱图; (b) 5%Ru/N-RHC_{0.5-873 K}的XPS全谱图；5%Ru/N-RHC_{x-873 K}样品的精细谱图; (c) Ru 3p; (d) N 1s

Figure 2 (a) XRD patterns of 5%Ru/N-RHC_{0.5-873 K} catalysts; XPS spectra of the 5%Ru/N-RHC_{0.5-873 K} samples: (b) survey, (c) Ru 3p, (d) N 1s

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图 3 不同三聚氰胺含量的5%Ru/N-RHC_{x-823 K}催化AB分解产氢反应中的脱氢速率

Figure 3 Dehydrogenation rate curve of AB hydrolysis over various 5% Ru/N-RHC_x_{-823 K} catalysts with different melamine contents

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图 4 不同煅烧温度下的5%Ru/N-RHC_0.5-y催化AB分解产氢反应中的脱氢速率

Figure 4 Dehydrogenation rate curve of AB hydrolysis over various 5%Ru/N-RHC_0.5-y catalysts obtained at different calcination temperatures

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图 5 不同Ru负载量的Ru/N-RHC_{0.5-873 K}催化剂在 298 K 催化 AB 水解反应中的脱氢速率

Figure 5 Dehydrogenation rate curve of AB hydrolysis over various Ru/N-RHC_{0.5-873 K} catalysts with different Ru loadings

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图 6 (a) 298 K时AB脱氢速率随AB浓度的变化；(b) AB脱氢速率与AB浓度的对数值

Figure 6 (a) Plots of hydrogen evolution rate for the AB hydrolysis with different AB concentrations at 298 K; (b) Logarithmic plot of hydrogen evolution rate versus AB concentration

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图 7 (a) 298 K时AB脱氢速率随催化剂含量的变化；(b) AB脱氢速率与催化剂质量的对数值

Figure 7 (a) Plots of hydrogen evolution rate for the AB hydrolysis with different catalyst concentrations at 298 K;(b) Logarithmic plot of hydrogen evolution rate versus the catalyst concentration

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图 8 有光时不同温度下5%Ru/N-RHC_{0.5-873 K} 催化AB脱氢速率（a）和阿伦尼乌斯方程：lnk与1000/T关系（b）；无光时不同温度下5%Ru/N-RHC_{0.5-873 K} 催化AB脱氢速率（c）和阿伦尼乌斯方程：lnk与1000/T关系（d）

Figure 8 AB dehydrogenation rate curves over the 5%Ru/N-RHC_{0.5-873 K} catalyst at different temperatures under light irradiation (a) and corresponding Arrhenius plot of lnk versus 1000/T (b)；AB dehydrogenation rate curves over the 5%Ru/N-RHC_{0.5-873 K} catalyst at different temperatures without light irradiation (c) and corresponding Arrhenius plot of lnk versus 1000/T (d)

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