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

doi:10.6023/A21030126

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (7): 885-902.DOI: 10.6023/A21030126 Previous Articles Next Articles

Review

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)

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

Cite this article

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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Fig. & Tab. 16

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]

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

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]

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]

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]

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]

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

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]

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]

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]

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]

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]

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]

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]

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]

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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