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化学进展 2020, Vol. 32 Issue (12): 1930-1951 DOI: 10.7536/PC200323 前一篇   后一篇

• 综述 •

氨硼烷催化水解制氢

姚淇露1, 杜红霞1, 卢章辉1,**()   

  1. 1 江西师范大学先进材料研究院/化学化工学院 南昌 330022
  • 收稿日期:2020-03-24 修回日期:2020-04-16 出版日期:2021-10-15 发布日期:2020-10-13
  • 通讯作者: 卢章辉
  • 作者简介:
    ** Corresponding author e-mail:
  • 基金资助:
    国家自然科学基金项目(No. 21763012); 国家自然科学基金项目(21802056); 江西省自然科学基金项目(No. 20192BAB203009); 江西师范大学青年英才项目资助
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Catalytic Hydrolysis of Ammonia Borane for Hydrogen Production

Qilu Yao1, Hongxia Du1, Zhang-Hui Lu1,**()   

  1. 1 Institute of Advanced Materials(IAM), College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China
  • Received:2020-03-24 Revised:2020-04-16 Online:2021-10-15 Published:2020-10-13
  • Contact: Zhang-Hui Lu
  • Supported by:
    the National Natural Science Foundation of China(No. 21763012); the National Natural Science Foundation of China(21802056); the Natural Science Foundation of Jiangxi Province of China(No. 20192BAB203009); and the Sponsored Program for Cultivating Youths of Outstanding Ability in Jiangxi Normal

氢气作为全球公认的清洁能源载体,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氢能应用面临最大的挑战之一。氨硼烷(NH3BH3,AB)具有非常高的储氢质量分数(19.6 wt%)和体积储氢密度(0.145 kgH2/L),因其在储氢和放氢性能方面的显著优势,被认为是一种颇具应用潜力的化学储氢材料。氨硼烷能够通过热解、醇解和水解放出氢气。其中,氨硼烷水解制氢可以通过催化剂进行可控放氢,且具有反应条件温和、不产生CO(易使催化剂中毒)等优点,被认为是一种安全高效和实用性强的制氢技术。本文简要介绍了氨硼烷的性质和合成,阐述了氨硼烷水解制氢的机理,综述了近年来氨硼烷水解制氢催化剂的研究进展,分析了碱对氨硼烷水解制氢的促进作用,并讨论了水解产物回收利用问题。

关键词： 化学储氢材料, 氨硼烷, 水解, 制氢, 催化剂

Hydrogen has attracted much attention as a globally accepted clean energy carrier. Currently, the search of safe and efficient hydrogen storage materials is one of the most difficult challenges for the transformation to hydrogen powered society as a long-term solution for a secure energy future. Ammonia borane(NH3BH3, AB) has been considered to be a promising chemical hydrogen storage material due to its high hydrogen capacity(19.6 wt%), high volumetric hydrogen density(0.145 kgH2/L), and remarkable advantages in hydrogen storage and dehydrogenation performance. Hydrogen stored in ammonia borane can be released via pyrolysis, methanolysis, and hydrolysis routes. Among them, hydrolysis of ammonia borane can be easily controlled and without CO produced(easy to poison the catalyst) in the presence of an appropriate catalyst under mild conditions, which seems to be the most safe, effective, and convenient route for hydrogen storage applications. In this review, the properties and synthesis of ammonia borane are briefly introduced. The mechanism of hydrogen production from ammonia borane is described. Meanwhile, the research progress in catalytic hydrolytic dehydrogenation of ammonia borane for chemical storage is significantly reviewed. Moreover, the promoting effect of alkali for this hydrolysis reaction is concisely analyzed and the recovery of hydrolysate is also discussed.

Contents

1 Introduction

2 Properties and synthesis of ammonia borane

2.1 Properties of ammonia borane

2.2 Synthesis of ammonia borane

3 Mechanism of catalytic ammonia borane hydrolysis

4 Metal catalysts for the hydrolysis of ammonia borane

4.1 Noble metal catalysts

4.2 Non-noble metal catalysts

4.3 Synergistic metal catalysts

4.4 Other catalysts

5 Promoting effect of alkali on catalytic ammonia borane hydrolysis

6 Regeneration of ammonia borane

7 Conclusion

Key words: chemical hydrogen storage material, ammonia borane, hydrolysis, hydrogen production, catalyst
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图1 金属催化剂催化氨硼烷制氢机理的示意图
Fig.1 The schematic diagram of metal catalyst for hydrogen generation from hydrolysis of AB
图2 (a) Pt/CNT催化剂的高分辨TEM图;(b)截断八面体的示意图;(c) Pt颗粒表面不同位置原子数量随颗粒尺寸变化的关系图;(d) 不同位置原子归一化的TOF随颗粒尺寸变化的关系图[50]
Fig.2 (a) Typical HRTEM image of Pt nanoparticle supported on CNT.(b) Schematic diagram of truncated cuboctahedron.(c) Plots of number of surface atoms per mole of Pt with Pt particle size of truncated cuboctahedron.(d) Plots of normalized TOF with Pt particle size[50]. Reprinted with permission from ref [50]. Copyright 2014, American Chemical Society
图3 不同类型催化剂催化氨硼烷水解制氢循环性能图[52]
Fig.3 Turnover frequency(TOF) values of different catalysts in successive runs for the hydrolysis of AB at 25 ℃(Pt/AB=0.0079)[52]. Reprinted with permission from ref [52]. Copyright 2016, Wiley-VCH
图4 Ru@SBA-15纳米催化剂制备示意图[72]
Fig.4 Schematic illustration of preparation of Ru@SBA-15 catalys[72]. Reprinted with permission from ref[72]. Copyright 2015, Rights Managed by Nature Publishing Group
图5 Ru@SiO 2催化剂(Ru负载量:6 wt%;[Ru]:0.5 mM)催化氨硼烷水解制氢性能图;插图是不同Ru负载量与时间关系图;(b) 不同金属负载量的Ru@SiO2催化剂的TEM图[73]
Fig.5 (a) Hydrogen generation from hydrolysis of AB(200 mM, 10 mL) by Ru@SiO 2 nanospheres(Ru loading=6 wt% and [Ru]=0.5 mM) at 298 K. The inset shows the reaction time versus the loading of ruthenium;(b) Representative TEM images of the Ru@SiO2 nanospheres with different Ru loadings[73]. Reprinted with permission from ref [73]. Copyright 2014, Elsevier
图6 MCN、Pd 67Ni 33与Pd 74Ni 26/MCN催化剂在室温条件下催化氨硼烷水解制氢性能图;插图是不同催化剂对应的TOF值图[79]
Fig.6 Time plots for hydrogen release from aqueous AB solution(200 mM, 5 mL) catalyzed by MCN, Pd 67Ni 33, and Pd 74Ni 26/MCN NCs at room temperature. Inset: the corresponding TOF values of the catalysts[79]. Reprinted with permission from ref [79]. Copyright 2018, Wiley-VCH
表1 不同贵金属催化剂催化氨硼烷水解制氢的催化性能对比
Table 1 Catalytic performance of noble metal catalysts for hydrogen generation from the hydrolysis of ammonia borane
Catalyst T/K n metal/ n AB TOF/min -1 E a/kJ·mol -1 ref
Commercial 20 wt% Pt/C RT 0.018 83.3 - 19
Pt/γ-Al 2O 3 RT 0.018 222.2 21 48
Pt@MIL-101 298 0.0029 413.8 - 49
Pt/CNTs 298 - 407.2 38 50
Pt@CeO 2 nanonecklace RT 0.018 133.3 - 51
Pt-CeO 2/rGO 298 0.0079 93.8 64.7 52
Pt 2/graphene 300 0.0011 2800 - 53
Pt@SiO 2 303 0.00245 158.6 53.9 74
Pt@PC-POP 303 - 104.33 56.42 85
Pt25@TiO 2 298 0.0016 311 - 86
Pt@h-mNSiO 2 298 0.0013 371.7 49.4 87
Rh/γ-Al 2O 3 RT 0.018 128 21 48
Rh/NaY 298 0.002 92 66.9 59
Rh/CeO 2 298 0.0008 2010 42.6 62
Rh/AC 298 0.0038 188 39.9 63
Rh/graphene 298 0.004 325 19.7 64
Rh/CNTs 298 0.0025 706 32 65
Rh@S-1-H 298 0.0011 699 75.5 66
In situ Rh/C 298 0.0114 1246 40.9 88
Rh@UiO-66 298 0.0056 219.8 38.4 89
Ru/γ-Al 2O 3 RT 0.018 55.5 23 48
Ru/Carbon black 298 0.0085 429.5 34.81 69
Ru/C-300 298 0.0034 643 38.7 70
Ru/Ce(OH)CO 3 298 0.0069 389.6 60.16 71
Ru@SBA-15 298 0.0025 231 34.8 72
Ru@SiO 2 298 0.002 200 38.2 73
Ru/MWCNT 298 0.00094 329 33 90
Ru/graphene 298 0.002 600 12.7 91
Ru/g-C 3N 4 298 0.0013 384.6 37.4 92
Metastable Ru 298 0.0025 21.8 27.5 93
Pd/RGO 298 0.004 6.25 51 76
Pd/MCN 298 0.03 125 57 79
Pd/SiO 2-CoFe 2O 4 298 0.0019 254 52 84
Ag/SBA-15 298 0.093 12 - 80
Ag/SiO 2-CoFe 2O 4 298 0.0028 264 53.4 82
图7 (a) Co/MIL-101-1-U,(b) Co/MIL-101-1,(c) Co/MIL-101-2-U,(d) Co/MIL-101-2催化剂的合成示意图[104]
Fig.7 Schematic illustration for the synthesis of four types of MIL-101-supported Co NPs: (a) Co/MIL-101-1-U;(b) Co/MIL-101-1;(c) Co/MIL-101-2-U;(d) Co/MIL-101-2[104]. Reprinted with permission from ref [104]. Copyright 2017, American Chemical Society
表 2 不同非贵金属催化剂催化氨硼烷水解制氢的催化性能对比
Table 2 Catalytic performance of non-noble metal catalysts for hydrogen generation from the hydrolysis of ammonia borane.
Catalyst T/K n metal/ n AB TOF/min -1 E a/kJ·mol -1 ref
In situ Fe NPs RT 0.12 3.12 - 94
Co/γ-Al 2O 3 RT 0.018 2.27 62 42
In situ Co NPs RT 0.04 44.1 - 95
Co/PEI-GO 298 0.11 39.9 28.2 103
Co/MIL-101-1-U 298 0.02 51.4 31.3 104
Co/NPCNW 298 0.075 7.29 25.4 105
Co@N-C-700 298 0.057 5.6 31 106
Co/HPC 323 0.11 2.94 32.8 107
Co/CTF 298 0.05 42.3 42.7 108
Co NCs@PCC-2a 298 0.07 90.1 - 109
Co/rGO 298 0.1 6.86 27.1 102
Co@C-N@SiO 2-800 298 - 8.4 36.1 109
G6-OH(Co 60) 298 0.013 10 50.2 110
Co-(CeO x ) 0.91 298 0.04 79.5 31.82 111
Ni/γ-Al 2O 3 RT 0.018 2.5 - 42
Ni/C 298 0.0425 8.8 28 119
Ni/SiO 2 298 0.0225 13.2 34 120
Ni/ZIF-8 RT 0.016 14.2 - 123
Ni@MSC-30 RT 0.016 30.7 - 124
NiMo/graphene 298 0.05 66.7 21.8 128
Ni-CeO x /graphene 298 0.08 68.2 28.9 135
Ni@3D-(N)GFs RT 0.009 41.7 - 113
Ni/CNT 298 - 26.2 32.3 115
Ni/PDA-CoFe 2O 4 298 0.017 7.6 50.8 116
Ni/Ketjenblack 298 0.13 7.5 66.6 118
Cu/γ-Al 2O 3 RT 0.018 0.23 - 42
Cu@Cu 2O 293 0.15 0.32 - 43
Zeolite confined Cu 298 0.013 1.25 51.8 137
Cu/CoFe 2O 4@SiO 2 298 0.0031 40 - 140
Cu/RGO 298 0.1 3.61 38.2 142
Cu@SiO 2 298 0.08 3.24 36 143
p(AMPS)-Cu 303 0.069 0.72 48.8 144
图8 不同催化剂催化氨硼烷水解制氢性能图[128]
Fig.8 TOF values of the different catalysts for hydrogen generation from hydrolysis of AB[128]. Reprinted with permission from ref [128]. Copyright 2016, Royal Society of Chemistry
图9 不同催化剂催化氨硼烷水解制氢性能图[135]
Fig.9 Hydrogen productivity vs. reaction time for hydrogen release from an aqueous AB solution(200 mM, 5 mL) catalyzed by different catalysts at 298 K( n Ni/ n AB=0.08)[135]. Reprinted with permission from ref[135]. Copyright 2018, Tsinghua University Press and Springer-Verlag GmbH Germany
图10 (a) 不同催化剂催化氨硼烷水解制氢性能图;(b)Cu/RGO催化剂的TEM图[142]
Fig.10 (a) Hydrogen generation from hydrolysis of AB in presence of different catalysts;(b) TEM image of Cu/RGO[142]. Reprinted with permission from ref[142]. Copyright 2014, Royal Society of Chemistry
图11 Cu@SiO 2催化剂催化氨硼烷和肼硼烷水解制氢循环性能图[143]
Fig.11 Percent of initial activity retained in the successive runs for the hydrolysis of AB and HB in the presence of Cu@SiO 2 catalyst at 298 K[143]. Reprinted with permission from ref[143]. Copyright 2014, Rights Managed by Nature Publishing Group
表 3 不同多金属协同催化剂催化氨硼烷水解制氢的催化性能对比
Table 3 Catalytic performance of synergistic metal catalysts for hydrogen generation from the hydrolysis of ammonia borane
Catalyst T/K n metal/ n AB TOF/min -1 E a/kJ·mol -1 ref
PtPd cNPs 298 0.002 50.02 57.3 152
PtPd sNPs 298 0.002 22.51 - 152
Pt 70Ru 30-NP 298 0.001 59.6 38.9 153
PdRh-PVP 298 0.003 1333 46.1 155
Ag 1Pd 4@UIO-66-NH 2 298 0.0125 90 51.77 149
PtNi@SiO 2 303 0.036 5.54 54.76 164
Ni 2Pt@ZiF-8 293 0.01 361.4 23.3 166
Pt-Co/dendrimer 293 0.01 303 28.8 168
PtCo 20/CNTs 298 - 675.1 a 42.5 169
RuNi/TiO 2 298 0.001 914 28.1 173
RuCo/γ-Al 2O 3 338 - 32.9 47 175
RuCu/γ-Al 2O 3 338 - 16.4 52 175
AuNi@MIL-101 RT 0.017 66.2 - 180
AuCo@MIL-101 RT 0.017 23.5 - 183
Ag-doped Ni/MIL-101 298 0.017 20.2 25 186
AgCo/PAMAM 298 0.033 15.84 35.66 188
Pd 67Ni 33/MCN 298 0.03 222.2 54.1 79
Ni 30Pd 70/rGO 298 0.01 28.7 45 189
Ni 3Pd 7/CS 298 0.024 187.5 35.32 191
Co 35Pd 65/C 298 0.024 22.7 27.5 192
Pd@Co@MIL-101 303 0.011 51 22 194
Fe 0.5Ni 0.5alloy 293 0.12 11.4 - 202
Fe 0.3Co 0.7 alloy 293 0.12 13.9 16.3 205
CuCo/graphene 293 0.02 9.18 - 212
Cu 0.5Co 0.5@SiO 2 298 0.08 4.26 24 213
CuCo@MIL-101-1-U 298 0.02 51.7 30.5 104
Cu 0.2Co 0.8/PDA-rGO 303 0.05 51.5 54.9 215
Cu 0.3Co 0.7@MIL-101 RT 0.034 19.6 - 218
Cu 0.72Co 0.18Mo 0.1 298 0.04 119.0 b 45 222
Cu 0.72Co 0.18Mo 0.1 298 0.04 46.0 - 222
Cu 0.8Co 0.2O-GO 298 0.024 70.0 45.5 237
Cu 0.33Fe 0.67 298 0.04 13.95 43.2 223
Cu 0.2Ni 0.8/MCM-41 298 0.05 10.7 38 224
CuNi/CMK-1 298 0.072 54.8 - 226
图12 一步原位晶种法形成Au@Co核壳纳米粒子的 (a)示意图和(b)溶液颜色变化照片[185]
Fig.12 (a) Schematic illustration,(b) color evolution in the formation process of Au@Co core-shell NPs via a one-step seeding-growth method at room temperature[185]. Reprinted with permission from ref [185]. Copyright 2010, American Chemical Society
图13 (a) Cu x Co 1- x @SiO 2催化剂催化氨硼烷水解制氢性能图;(b) Cu 0.5Co 0.5@SiO 2催化剂的TEM图[213]
Fig.13 (a) Cu x Co 1- x @SiO 2 core-shell nanospheres with different x values under an ambient atmosphere at 298 K;(b) TEM image of Cu 0.5Co 0.5@SiO2 [213]. Reprinted with permission from ref[213]. Copyright 2015, American Chemical Society
图14 不同催化剂催化氨硼烷水解制氢性能图;插图是原位合成Cu0.33Fe 0.67纳米合金的的照片[223]
Fig.14 Hydrogen generation from the hydrolysis of AB in the presence of different metal nanocatalysts(metal/AB=0.04). The insert shows photographs of the catalytic hydrolysis of AB via in situ synthesized Cu 0.33Fe 0.67 nanoalloy[223]. Reprinted with the permission from ref [223]. Copyright 2013, Elsevier
图15 Cu 0.72Co 0.18Mo 0.1催化剂在添加NaOH、KOH、Na 2CO 3、NH 4Cl、CH 3COONH 4和NH 3·H 2O条件下催化氨硼烷水解制氢性能图[222]
Fig.15 Hydrogen generation from the hydrolysis of AB with the addition of NaOH, KOH, Na 2CO 3, NH 4Cl, CH 3COONH 4 and NH 3·H 2O catalyzed by Cu 0.72Co 0.18Mo 0.1 NPs at 298 K[222]. Reprinted with the permission from ref[ 222]. Copyright 2018, Royal Society of Chemistry
图16 氨硼烷水解副产物再生使用示意图
Fig.16 Ammonia borane regeneration cycle from byproducts of hydrolysis
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摘要

氨硼烷催化水解制氢