水合肼分解产氢催化剂研究进展

doi:10.6023/A21030126

化学学报 ›› 2021, Vol. 79 ›› Issue (7): 885-902.DOI: 10.6023/A21030126 上一篇下一篇

综述

水合肼分解产氢催化剂研究进展

张安琪, 姚淇露, 卢章辉^*()

江西师范大学化学化工学院功能有机小分子教育部重点实验室南昌 330022

投稿日期:2021-03-31 发布日期:2021-05-11
通讯作者: 卢章辉

作者简介:

张安琪, 1997年出生, 2019年本科毕业于巢湖学院, 随后加入江西师范大学卢章辉教授课题组攻读硕士学位, 主要研究方向为纳米材料的可控合成及其在能源与催化领域的应用.

姚淇露, 江西师范大学先进材料研究院助理研究员. 2017年于江西师范大学获得理学博士学位. 毕业后留校进入先进材料研究院工作. 主要研究方向为纳米材料的可控合成及其在能源与催化领域的应用. 以第一作者或通讯作者在国内外知名期刊发表SCI收录论文20余篇; 获授权发明专利5项; 获江西省自然科学奖一等奖(第二完成人).

卢章辉, 江西师范大学化学化工学院教授/博导, 江西省赣鄱英才555工程领军人才. 2011年于日本国立神户大学获得博士学位, 2008年10月至2011年9月, 在日本产业技术综合研究所从事研究, 2011年10月至今在江西师范大学工作. 主要从事能源催化研究, 在国内外知名期刊发表SCI收录论文110篇, 被引4500余次, 获江西省自然科学奖一等奖(第一完成人).

基金资助:
国家自然科学基金(21763012); 江西师范大学研究生创新基金(YJS2020020)

Recent Progress on Catalysts for Hydrogen Evolution from Decomposition of Hydrous Hydrazine

Anqi Zhang, Qilu Yao, Zhang-Hui Lu()

Key Laboratory of Functional Small Molecules for Ministry of Education, School of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China

Received:2021-03-31 Published:2021-05-11
Contact: Zhang-Hui Lu
Supported by:
National Natural Science Foundation of China(21763012); Post-graduate’s Innovation Fund Project of Jiangxi Normal University(YJS2020020)

文章分享

摘要/Abstract

氢气作为21世纪最具发展前景的清洁能源, 一直备受关注. 寻找安全高效的储氢材料以转型到氢能社会是当前面临的最大挑战之一. 水合肼(N₂H₄•H₂O)具有高含氢量(w=8.0%), 完全分解产氢副产物仅为氮气和水, 被视为一种极具应用潜力的液相化学储氢材料. 开发高效、高选择性的催化剂以催化水合肼完全分解, 是研究水合肼分解产氢的关键. 本综述总结了水合肼分解产氢催化剂的设计、合成及其催化性能. 简要分析了肼分解的机理. 此外, 讨论了提高水合肼分解产氢催化剂的选择性和活性的策略, 比如添加强碱助剂/碱性载体、形成合金、降低金属催化剂的结晶度、减小粒子尺寸、以及增强金属与载体相互作用. 本研究进展可以为设计合成具有更高活性的氮基氢化物产氢催化剂提供指导和思路.

关键词: 化学储氢材料, 水合肼, 产氢, 催化剂

Hydrogen with remarkable energy density has attracted much attention as the green, sustainable chemical energy carrier and a substitute for traditional fossil fuels. The discovery of safe and efficient hydrogen storage materials for the transition to a hydrogen energy society is one of the biggest challenges for hydrogen energy applications today. Hydrous hydrazine (N₂H₄•H₂O), with its high hydrogen content (w=8.0%) and the advantage of CO-free hydrogen production, has significant advantages in hydrogen storage and release and is considered as a promising liquid-phase chemical hydrogen storage material. The development of efficient and highly selective catalysts is the key to release hydrogen from the decomposition of hydrous hydrazine. In the past decade, a lot of catalysts have been developed to improve the kinetic properties for hydrogen generation. In this review, we focus on the recent progress on catalyst design, synthesis and catalytic performance of the catalyst in hydrogen production from the selective decomposition of hydrous hydrazine. Ir, Rh and Ni monometallic catalysts were found to be very active toward the dehydrogenation of hydrazine. Among all the catalysts investigated, supported Pt-Ni, Rh-Ni and Pt-Co catalysts showed the highest activity. The mechanism of hydrazine decomposition was briefly analyzed. The cleavage of the N―H bond of N₂H₄ will facilitate the formation of H₂ and N₂, while N―N bond cleavage will result in the formation of NH₃ and N₂. In addition, we reviewed and discussed the strategies for promoting H₂ selectivity and activity of catalysts, such as the addition of strong base and/or alkaline carrier, formation of metal alloys, reduction of metal crystallinity and particle size, as well as the enhancement of the interaction between metal and support. The progress of this research may provide guidance for obtaining more active catalysts toward hydrogen production from nitrogen-based hydrides.

Key words: chemical hydrogen storage material, hydrazine hydrate, hydrogen production, catalyst

引用此文

张安琪, 姚淇露, 卢章辉. 水合肼分解产氢催化剂研究进展[J]. 化学学报, 2021, 79(7): 885-902.

Anqi Zhang, Qilu Yao, Zhang-Hui Lu. Recent Progress on Catalysts for Hydrogen Evolution from Decomposition of Hydrous Hydrazine[J]. Acta Chimica Sinica, 2021, 79(7): 885-902.

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图/表 16

图1. 25 ℃时, 无碱条件下, 不同金属纳米颗粒(nmetal/nN2H4=1∶10)在水溶液中催化水合肼分解产氢, 生成的气体与时间的关系图. 插图为Rh(0)纳米颗粒的透射电子显微镜(TEM)图和相应的选区电子衍射(SAED)图(比例尺寸为20 nm)[17]

Figure 1. Time course plots for the decomposition of hydrazine in aqueous solutions in the presence of different metal NPs (nmetal/nN2H4=1∶10) at 25 ℃. The inset shows a transmission electron microscope (TEM) image of Rh(0) NPs and the corresponding selected area electron diffraction (SAED) pattern. Scale bar, 20 nm[17]

Catalyst	T/℃	TOF/h^-1	Hydrogen selectivity/%	Ref.
Pt	25	—	0	[17]
Pd	25	—	0	[17]
Cu	25	—	0	[17]
Fe	25	—	0	[17]
Ni	25	—	0	[17]
Co	25	—	7	[17]
Ru	25	—	7	[17]
Ir	25	—	7	[17]
Rh	25	—	43.8	[17]
Ni-Al₂O₃-HT	30	2.0^a	93	[18]
Ni/Al₂O₃-IMP	30	2.86^a^,^b	66	[18]
Ni-CeO₂	30	51.6	99	[19]
Raney Ni-300	30	162^a^,^b	99	[27]
Ni/CeO₂	50	34	100	[20]
Ni@TNTs	60	96^a	100	[25]
Rh	70	—	34	[27]
Ir/Al₂O₃	>200	—	100	[15]
Ir/γ-Al₂O₃	>200	—	100	[16]
Ni-CeO₂@SiO₂	70	219.5	100	[23]

表1. 单金属催化剂催化水合肼分解制氢的催化性能对比

Table 1. Comparison of catalytic performance of monometallic catalysts for hydrogen production from decomposition of hydrous hydrazine

图2. Ni, Ni/CeO2-IMP和Ni-0.080CeO2催化剂的结构模型以及催化水合肼产氢性能对比图[19]

Figure 2. Structure model of Ni, Ni/CeO2-IMP and Ni-0.080CeO2 catalysts and the comparison of catalytic performance of hydrogen production from hydrazine hydrate[19]

图3. Ni-CeO2@SiO2纳米催化剂的(a) SEM图, (b, c) TEM图, (d) 高角环形暗场像-扫描透射电子显微镜(HAADF-STEM)图及相应的(e~j) 扫描透射电子显微镜能谱(STEM-EDX)面扫图[23]

Figure 3. (a) SEM image, (b, c) TEM images, (d) high-angle annular dark-field-scanning transmission electron microscope (HAADF-STEM) image, and (e~j) energy dispersive X-ray (EDX) mapping of Ni-CeO2@SiO2 catalyst[23]

图4. 雷尼镍(Raney Ni-300)催化剂的(a) SEM图; (b) 在30 ℃, NaOH浓度为0.5 mol•L-1时, 分解水合肼(0.16 mol•L-1)的循环实验图[27]

Figure 4. (a) SEM image of Raney Ni catalyst; (b) the recycling test of Raney Ni‐300 with NaOH (0.5 mol•L-1) for hydrous hydrazine (0.16 mol•L-1) decomposition, carried out at 30 ℃[27]

Catalyst	T/℃	TOF/h^-1	Hydrogen selectivity/%	Ref.
Ni_0.6Pd_0.4	25	—	7	[95]
Ni₃₀Fe₃₀Pd₄₀	25	4.0^b	100	[97]
Ni_0.95Ir_0.05-CTAB	25	3.08^b	100	[90]
Ni_0.6Pd_0.4	25	20^a^,^b	100	[96]
NiRh@rGO	25	24.5^b	100	[38]
CoIr_0.081/γ-Al₂O₃	25	27.76	100	[100]
Ni_0.9Pt_0.1/Ce₂O₃	25	28.1^a	100	[67]
NiPtRh/La₂O₃	25	45.9^a	100	[88]
Rh/Ni@SiO₂	25	66^a	99.4	[52]
Ni₆₄Pt₃₆/MIL-96	25	114.3^a	100	[84]
(Ni₃Pt₇)_0.5-(MnO _x)_0.5/NPC-900	25	120^a	100	[85]
NiPt/NH₂-MIL-101	25	137^a	100	[86]
Ni₆₀Pt₄₀-SF-I	25	150^a	100	[62]
Co_0.65Pt_0.30(CeO _x)_0.05	25	194.8^a	72.1	[98]
Ni_0.7Pt_0.3P/rGO	25	224^a	100	[103]
NiIr_0.059/Al₂O₃	30	12.4^a	99	[91]
Ni_0.2Rh_0.8@CeO _x/rGO	30	36.4^b	100	[47]
Ni_0.9Pt_0.1/MIL-101	30	140^a	100	[81]
Ni₄₅Rh₅₅/Ce(OH)CO₃	30	150^a	100	[48]
Ni₄₀Pt₆₀-CNDs	30	170^a	100	[80]
Ni₆₀Pt₄₀/CeO₂	30	293	100	[66]
Ni_0.58Pt_0.42/grapheme	30	434^a	100	[76]
CoPt/La(OH)₃	30	734.2^a	100	[99]
Ni_0.4Pt_0.6/PDA-rGO	30	903^a	100	[75]
Ni_0.9Rh_0.1	50	0.045^b	100	[35]
Ni_0.99Pt_0.01	50	5.7^b	100	[61]
Ni_0.6Pd_0.4	50	6.3^b	82	[95]
NiRh@ZIF-8	50	140^a	100	[55]
Ni₃Rh₇/NPC-900	50	156^a	100	[56]
NiPt/C	50	210^a	100	[63]
Ni@Ni-Pt/La₂O₃	50	312^a	100	[69]
Ni₄₂Rh₅₈@MIL-101	50	344^a	100	[57]
Ni_0.2Rh_0.8/MIL-101	50	428.6	100	[59]
NiIr/MIL-101	50	464^a	100	[94]
RhNiP/rGO	50	471^a	100	[102]
NiIr/La₂O₂CO₃	50	487^a	100	[93]
Rh_0.5(MoO _x)_0.5	50	750^a	100	[105]
Ni_0.6Pt_0.4-MoO _x	50	822^a	100	[106]
Rh_92.6P_7.4/rGO	50	843.9^a	100	[101]
Ni_0.2Rh_0.8/Mxene	50	857^a	100	[45]
NiPt/DT-Ti₃C₂T _x	50	1220^a	100	[89]
Ni_0.4Pt_0.6@ZrO₂/C/rGO	50	1920^a	100	[73]
CoPt/La(OH)₃	50	2400^a	100	[99]

Catalyst	T/℃	TOF/h^-1	Hydrogen selectivity/%	Ref.
Ni_0.6Pd_0.4	25	—	7	[95]
Ni₃₀Fe₃₀Pd₄₀	25	4.0^b	100	[97]
Ni_0.95Ir_0.05-CTAB	25	3.08^b	100	[90]
Ni_0.6Pd_0.4	25	20^a^,^b	100	[96]
NiRh@rGO	25	24.5^b	100	[38]
CoIr_0.081/γ-Al₂O₃	25	27.76	100	[100]
Ni_0.9Pt_0.1/Ce₂O₃	25	28.1^a	100	[67]
NiPtRh/La₂O₃	25	45.9^a	100	[88]
Rh/Ni@SiO₂	25	66^a	99.4	[52]
Ni₆₄Pt₃₆/MIL-96	25	114.3^a	100	[84]
(Ni₃Pt₇)_0.5-(MnO _x)_0.5/NPC-900	25	120^a	100	[85]
NiPt/NH₂-MIL-101	25	137^a	100	[86]
Ni₆₀Pt₄₀-SF-I	25	150^a	100	[62]
Co_0.65Pt_0.30(CeO _x)_0.05	25	194.8^a	72.1	[98]
Ni_0.7Pt_0.3P/rGO	25	224^a	100	[103]
NiIr_0.059/Al₂O₃	30	12.4^a	99	[91]
Ni_0.2Rh_0.8@CeO _x/rGO	30	36.4^b	100	[47]
Ni_0.9Pt_0.1/MIL-101	30	140^a	100	[81]
Ni₄₅Rh₅₅/Ce(OH)CO₃	30	150^a	100	[48]
Ni₄₀Pt₆₀-CNDs	30	170^a	100	[80]
Ni₆₀Pt₄₀/CeO₂	30	293	100	[66]
Ni_0.58Pt_0.42/grapheme	30	434^a	100	[76]
CoPt/La(OH)₃	30	734.2^a	100	[99]
Ni_0.4Pt_0.6/PDA-rGO	30	903^a	100	[75]
Ni_0.9Rh_0.1	50	0.045^b	100	[35]
Ni_0.99Pt_0.01	50	5.7^b	100	[61]
Ni_0.6Pd_0.4	50	6.3^b	82	[95]
NiRh@ZIF-8	50	140^a	100	[55]
Ni₃Rh₇/NPC-900	50	156^a	100	[56]
NiPt/C	50	210^a	100	[63]
Ni@Ni-Pt/La₂O₃	50	312^a	100	[69]
Ni₄₂Rh₅₈@MIL-101	50	344^a	100	[57]
Ni_0.2Rh_0.8/MIL-101	50	428.6	100	[59]
NiIr/MIL-101	50	464^a	100	[94]
RhNiP/rGO	50	471^a	100	[102]
NiIr/La₂O₂CO₃	50	487^a	100	[93]
Rh_0.5(MoO _x)_0.5	50	750^a	100	[105]
Ni_0.6Pt_0.4-MoO _x	50	822^a	100	[106]
Rh_92.6P_7.4/rGO	50	843.9^a	100	[101]
Ni_0.2Rh_0.8/Mxene	50	857^a	100	[45]
NiPt/DT-Ti₃C₂T _x	50	1220^a	100	[89]
Ni_0.4Pt_0.6@ZrO₂/C/rGO	50	1920^a	100	[73]
CoPt/La(OH)₃	50	2400^a	100	[99]

表2. 含贵金属催化剂催化水合肼分解制氢的催化性能对比

Table 2. Comparison of the catalysts containing noble metals for hydrogen production from decomposition of hydrous hydrazine

表2. 含贵金属催化剂催化水合肼分解制氢的催化性能对比

Table 2. Comparison of the catalysts containing noble metals for hydrogen production from decomposition of hydrous hydrazine

Catalyst	T/℃	TOF/h^-1	Hydrogen selectivity/%	Ref.
NiCoP_1.5/SiO₂	25	1.71	100	[123]
NiCo/NiO-CoO _x	25	5.49	100	[124]
Ni_1.5Fe/(MgO)_2.5	25	24^b	99	[112]
Co₄N-Al₂O₃ (HT)	50	—	100	[125]
NiFe/CeO₂	50	5.73	99	[113]
Ni_0.6Fe_0.4Mo	50	28.8	100	[120]
CuNiMo	50	38.7	100	[109]
CuNi/CeO₂	50	1450^a	100	[122]
Ni₃Fe-(CeO _x)_0.15/rGO	55	56.8^a	100	[114]
Cu_0.5Ni_0.5/MCNS	60	21.8	100	[121]
NiFe	70	6.3^a^,^b	100	[111]
Cu@Fe₅Ni₅	70	20^b	100	[119]
Ni₄Mo@Cu₂O	70	71.4	100	[128]
NiFe/LaZrO₂	70	100.3^a	100	[115]
NiFe/NdZrO₂	70	103.7^a	100	[115]
NiFe/CeZrO₂	70	119.2^a	100	[115]
Ni₃Fe-(CeO _x)_0.15/rGO	70	126.2^a	100	[114]
Ni_0.9Fe_0.1-Cr₂O₃	70	893.5^a	100	[116]

表3. 非贵金属催化剂催化水合肼分解制氢的催化性能对比

Table 3. Catalytic activity of supported Co-, Cu-, Fe- and NiFe- based catalysts for hydrogen production from decomposition of hydrous hydrazine

图5. Rh4Ni纳米催化剂的(a) TEM图, (b) 高分辨透射电子图像(HRTEM)(插图: SAED图), (c) HAADF-STEM图(插图: 相应的EDS光谱图), (d) X射线衍射分析(XRD)图. (e) 室温下, 无碱条件下, Rh4Ni (nRh/nN2H4=1∶10)纳米催化剂催化水合肼(0.5 mol•L-1)分解的氢选择性以及相关的TEM 图[34]

Figure 5. (a) TEM image, (b) high resolution transmission electron microscope (HRTEM) image (inset: the corresponding SAED pattern), (c) HAADF-STEM image with the corresponding (assigned as *) EDS spectrum (Cu signals in EDS are from Cu grids), and (d) X-ray diffraction (XRD) profile of Rh4Ni nanocatalyst. (e) Hydrogen selectivity in hydrous hydrazine (0.5 mol•L-1) decomposition catalyzed by Rh4Ni with nRh/nN2H4=1∶10 at room temperature (The inset shows a TEM image of Rh4Ni nanocatalyst)[34]

图6. 25 ℃时, Ni, Pt和Ni1-xPtx (x=0.03~0.74)纳米催化剂催化水合肼(0.5 mol•L-1)分解制氢的氢气选择性对比图[60]

Figure 6. Hydrogen selectivities in the decomposition of hydrazine (0.5 mol•L-1) catalyzed by Ni, Pt, and Ni1-xPtx (x=0.03~0.74) nanocatalysts at 25 ℃[60]

图7. (a) 八面体PtNi/C纳米催化剂的HRTEM图, (b) 肼在Pt-Ni(111)表面选择性分解的示意图[63]

Figure 7. (a) HRTEM image of an octahedral PtNi/C nanocatalyst, (b) illustration of the selective hydrazine decomposition on the Pt-Ni(111) surface[63]

图8. (a) Ni/meso-CeO2和(b) Ni@Ni-Ir/meso-CeO2合成示意图; Ni@Ni-Ir/meso-CeO2纳米催化剂的(c) TEM图(插图: SAED图), (d) HRTEM图[91]

Figure 8. Schematic illustration of the synthesis of (a) Ni/meso‐CeO2 catalyst and (b) Ni@Ni-Ir/meso‐CeO2 catalyst; (c) TEM image (the upper inset is the corresponding SAED pattern) and (d) HRTEM image of Ni@Ni-Ir/meso-CeO2 [91]

图9. NiIr0.059/Al2O3催化剂在不同温度下还原的结构模型, 以及在反应温度为30 ℃时, 不同温度下还原的NiIr0.059/Al2O3催化剂催化水合肼分解的选择性和反应速率的对比图[92]

Figure 9. Structure model of NiIr0.059/Al2O3 catalyst reduced at different temperatures, and the comparison of selectivity and reaction rate for hydrous hydrazine decomposition at 30 ℃ of NiIr0.059/Al2O3 catalyst reduced at different temperatures[92]

图10. 50 ℃时, NaOH浓度为3.5 mol•L-1条件下, 由不同形貌的CoPt/La(OH)3纳米催化剂催化水合肼(400 mmol/mL, 5 mL)脱氢生成的气体与时间的关系图(nCoPt/nN2H4·H2O=0.05)[99]

Figure 10. Time course plots for dehydrogenation of N2H4 (400 mmol/mL, 5 mL) over CoPt NPs supported by shape-controlled La(OH)3 in the presence of NaOH (3.5 mol•L-1) at 50 ℃ (nCoPt/nN2H4·H2O=0.05)[99]

图11. 70 ℃时, NaOH浓度为0.5 mol•L-1条件下, 单金属(Fe、Co、Ni和Cu)和双金属(FeCo、NiFe、FeCu、NiCo、CoCu和NiCu)纳米催化剂催化水合肼(0.5 mol•L-1)分解产氢的氢气选择性对比图[111]

Figure 11. Comparative hydrogen selectivity in the decomposition of hydrous hydrazine (0.5 mol•L-1) to hydrogen in the presence of monometallic (Fe, Co, Ni and Cu) and bimetallic (FeCo, NiFe, FeCu, NiCo, CoCu and NiCu) nanocatalysts at 70 ℃[111]

图12. 50 ℃时, 浓度为0.5 mol•L-1的N2H4•H2O和2 mol•L-1的NaOH组成的4 mL溶液在(a) NiMoB(或NiB)或者(b) NiMoB-La(OH)3催化剂催化作用下产生的气体与时间的关系图[126]

Figure 12. Time course profiles of the system composed of 4 mL of 0.5 mol•L-1 N2H4•H2O+2 mol•L-1 NaOH solution catalyzed by (a) NiMoB (or NiB) or (b) NiMoB-La(OH)3 catalysts at 50 ℃ [126]

图13. 按照H2NNH2/N2+2H2途径的肼分解机理图

Figure 13. Mechanistic decomposition of hydrazine by the pathway: H2NNH2/N2+2H2

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水合肼分解产氢催化剂研究进展

Recent Progress on Catalysts for Hydrogen Evolution from Decomposition of Hydrous Hydrazine

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