无机材料学报 ›› 2020, Vol. 35 ›› Issue (7): 809-816.DOI: 10.15541/jim20190502 CSTR: 32189.14.10.15541/jim20190502
所属专题: 能源材料论文精选(四):光催化与电催化(2020)
收稿日期:2019-09-30
									
				
											修回日期:2019-12-28
									
				
									
				
											出版日期:2020-07-20
									
				
											网络出版日期:2020-03-03
									
			作者简介:张翊青(1995-), 女, 硕士研究生. E-mail: zhangyq95@163.com基金资助:
        
               		ZHANG Yiqing,ZHANG Shujuan,WAN Zhengrui,MO Han,WANG Niangui( ),ZHOU Liqun(
),ZHOU Liqun( )
)
			  
			
			
			
                
        
    
Received:2019-09-30
									
				
											Revised:2019-12-28
									
				
									
				
											Published:2020-07-20
									
				
											Online:2020-03-03
									
			Supported by:摘要:
开发高效廉价的催化剂对于清洁能源经济至关重要, 将氨硼烷的催化水解用于氢能源开发前景广阔。本工作首先采用简单回流法制备BiVO4纳米片, 再通过浸渍还原法制备出Ru/Fe不同摩尔比的RuFe@BiVO4催化剂, 并在室温下用于催化氨硼烷水解产氢。通过比较载体BiVO4、Ru@BiVO4、Fe@BiVO4、RuFe@BiVO4以及无载体的RuFe纳米粒子的催化产氢速率发现, 在所有的催化剂中, Ru1Fe0.1@BiVO4具有最高的催化活性, 非贵金属Fe能显著增强Ru的催化性能, 这与RuFe之间强的电子效应以及RuFe纳米粒子与载体BiVO4间的双功能效应密切相关, 其活化能(Ea)为43.7 kJ·mol-1, 转化频率(TOF)为205.4 molH2·molRu·min-1。
中图分类号:
张翊青,张淑娟,万正睿,莫晗,王念贵,周立群. RuFe纳米粒子修饰片状BiVO4协同催化氨硼烷水解产氢[J]. 无机材料学报, 2020, 35(7): 809-816.
ZHANG Yiqing,ZHANG Shujuan,WAN Zhengrui,MO Han,WANG Niangui,ZHOU Liqun. RuFe Nanoparticles Modified Sheet-like BiVO4 : High-efficient Synergistic Catalyst for Ammonia Borane Hydrolytic Dehydrogenation[J]. Journal of Inorganic Materials, 2020, 35(7): 809-816.
 
																													图1 BiVO4、Ru@BiVO4、Fe@BiVO4、Ru1Fe0.1@BiVO4和五次循环后Ru1Fe0.1@BiVO4的XRD图谱
Fig. 1 XRD patterns of BiVO4, Ru@BiVO4, Fe@BiVO4, Ru1Fe0.1@BiVO4 and Ru1Fe0.1@BiVO4 after five cycles
 
																													图2 BiVO4(A, B)、Ru1Fe0.1@BiVO4(C)和RuFe纳米粒子(E)的TEM照片; Ru1Fe0.1@BiVO4(D)、RuFe纳米粒子(F)的粒径分布图
Fig. 2 TEM images of BiVO4 (A, B), Ru1Fe0.1@BiVO4 (C) and RuFe NPs (E); particle size distributions of Ru1Fe0.1@BiVO4 (D) and RuFe NPs (F)
| Catalyst | Initial ratio of Ru : Fe | Actual ratio of Ru : Fe | Actual Ru loading/wt% | 
|---|---|---|---|
| RuFe@BiVO4 | 1 : 0.10 | 1 : 0.12 | 4.21 | 
表1 RuFe@BiVO4催化剂中元素的ICP-AES分析结果
Table 1 ICP-AES analyses results of RuFe@BiVO4 catalyst
| Catalyst | Initial ratio of Ru : Fe | Actual ratio of Ru : Fe | Actual Ru loading/wt% | 
|---|---|---|---|
| RuFe@BiVO4 | 1 : 0.10 | 1 : 0.12 | 4.21 | 
 
																													图6 不同催化剂对AB水解产氢速率图
Fig. 6 Plots of n(H2)/n(AB) vs. time from the hydrolysis of AB (18.5 mg) (A) Catalysts with the same nanoparticles loadings; (B) Ru1Fex NPs; (C) Ru1Fex@BiVO4 ; (D) Catalysts with different supporters
 
																													图8 温度对Ru1Fe0.1@BiVO4催化水解氨硼烷的影响曲线(A)及其相应的阿伦尼乌斯图(B), 催化剂五次循环稳定性(C)
Fig. 8 Plots of n(H2)/n(AB) vs. time for the hydrolysis of AB catalyzed by Ru1Fe0.1@BiVO4 at different temperatures(A) and corresponding Arrhenius plots (B), and cycling test for the Ru1Fe0.1@BiVO4 within five cycles (C)
| Catalyst | TOF/(molH2?molRu?min-1) | Ea/(kJ?mol-1) | Ref. | 
|---|---|---|---|
| Ru NPs | 26.7 | 66.5 | [ | 
| RuCu(1 : 1)/γ-Al2O3 | 16.4 | 52 | [ | 
| RuCo(1 : 11)/γ-Al2O3 | 32.9 | 47.0 | [ | 
| RuCuCo@MIL-101 | 241.2 | 48.0 | [ | 
| Ru@g-C3N4 | 313.0 | 37.4 | [ | 
| RuCu/graphene | 135.0 | 30.6 | [ | 
| Ru1Fe0.1@BiVO4 | 205.4 | 43.7 | This study | 
表2 不同钌基催化剂用于AB水解脱氢的催化活性
Table 2 Catalytic activities of different Ru-based catalysts used for the hydrolytic dehydrogenation of AB
| Catalyst | TOF/(molH2?molRu?min-1) | Ea/(kJ?mol-1) | Ref. | 
|---|---|---|---|
| Ru NPs | 26.7 | 66.5 | [ | 
| RuCu(1 : 1)/γ-Al2O3 | 16.4 | 52 | [ | 
| RuCo(1 : 11)/γ-Al2O3 | 32.9 | 47.0 | [ | 
| RuCuCo@MIL-101 | 241.2 | 48.0 | [ | 
| Ru@g-C3N4 | 313.0 | 37.4 | [ | 
| RuCu/graphene | 135.0 | 30.6 | [ | 
| Ru1Fe0.1@BiVO4 | 205.4 | 43.7 | This study | 
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