RESEARCH PROGRESS IN AMMONIA DECOMPOSITION OF IRON SERIES METAL CATALYSTS ASSISTED BY PLASMA
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摘要: 氢能作为一种零碳二次能源被广泛应用于各种工业领域. 氨作为一种储氢载体, 具有储氢量高(17.6 wt%)、能量密度高和易液化等特点, 其分解产物只有氢气和氮气, 符合国家“碳达峰, 碳中和”的战略发展方向. 但是氨分解的活化能高, 反应条件较为苛刻. 因此, 开发安全、高效、低成本的氨分解制氢技术对于氢能发展具有重要意义. 文章首先阐明了氨分解反应的基本原理, 介绍了铁系金属催化剂催化NH3分解制氢的研究进展, Fe, Co和Ni基催化剂的NH3分解活性较高, 因为其金属−氮的结合能适中, 之后从调控活性金属中心出发, 通过加入第二金属、调控形貌、缺陷/掺杂、构建金属−载体相互作用等方面设计提高氨分解的活性, 并采用多种表征方法揭示催化剂的构效关系. 除铁系催化剂外, 还重点介绍了提高氨分解效率的等离子体技术, 回顾了等离子体的原理、种类、作用机制以及在辅助催化氨制氢方面的协同效应. 文章综述了催化NH3分解的反应机理, 介绍了目前氨分解制氢催化剂设计的最新进展, 总结了提高NH3分解制氢的策略, 强调了等离子体在辅助催化NH3分解的优势. 对于今后氨分解制氢催化剂的开发和应用具有一定的参考价值, 期望为未来氨制氢的技术发展和工业化应用提供新思路.Abstract: Hydrogen energy is widely used in various industrial fields as a zero-carbon secondary energy source. As a hydrogen storage carrier, ammonia has the advantages of high hydrogen storage capacity (17.6 wt%), high energy density and easy liquefaction, and its decomposition products are only hydrogen and nitrogen, which is in line with the national strategic development direction of “carbon peak, carbon neutrality”. However, the activation energy of ammonia decomposition is high and the reaction conditions are harsh. Therefore, the development of safe, efficient and cheap ammonia decomposition hydrogen production technology is crucial for the development of hydrogen energy. In this paper, the basic principle of ammonia decomposition reaction is explained, and the research work of NH3 decomposition to hydrogen production catalyzed by various metal catalysts is introduced. Fe, Co and Ni based catalysts show higher NH3 decomposition activity because of their moderate metal-nitrogen binding energy. Beginning from the regulation of active metal centers, the researchers designed to improve the activity of ammonia decomposition by adding secondary metals, regulating morphology, defects/doping, constructing metal-carrier interactions, etc. The many characterization methods were used to reveal the structure-activity relationship of catalysts. In addition to the iron series catalysts, this paper also focuses on the plasma technology to improve the efficiency of ammonia decomposition and reveals the principle, types, mechanism of plasma and the synergistic effect in auxiliary catalytic ammonia hydrogen production. In this paper, the latest work in the design of ammonia decomposition catalyst for hydrogen production is introduced and the strategies for improving NH3 decomposition for hydrogen generation are summarized. The advantages of plasma-assisted NH3 decomposition are emphasized. This paper has certain reference value for the development and application of ammonia decomposition hydrogen generation catalysts, in order to provide a new idea for the development of ammonia hydrogen production technology and industrial application in the future.
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Key words:
- ammonia /
- hydrogen /
- hydrogen storage carrier /
- plasma /
- catalyst
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表 1 Fe基催化剂氨分解活性对比
Table 1. The comparison of catalytic activity over Fe based catalysts for NH3 decomposition
Fe loading/wt% Catalyst T/°C GHSV/(mL·gcat−1·h−1) NH3 conv./% H2 formation rate/(mmol·gFe−1·min−1) Ref. 5 Fe/MWCNTs 600 36000 45 — [10] 2.5 Fe/CNFs 600 18000 38.8 5.2 [11] 3.5 Fe/CNFs 600 6500 51.3 — [12] 3.5 Fe/CNFs/mica 600 6500 99 — [12] 2.5 Fe2O3/CMK-5 600 7500 97 — [13] 3.4 Fe-CNFs/CMFs 600 12000 100 4.3 [14] 34 Fe-BTC@400 500 30000 35 11 [15] 5% Fe/MS-H 700 30000 97 32 [16] — N-Mg5.3FeOm 680 150000 97.8 9.83 [17] 16.2 MRM-2-C900@700 700 120000 98.8 121.5 [18] — RMR-700 700 72000 95 72 [19] 
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表 2 Co基催化剂氨分解活性对比
Table 2. The comparison of catalytic activity over Co based catalysts for NH3 decomposition
Co loading/wt% Catalyst T/°C GHSV/(mL·gcat−1·h−1) NH3 conv./% H2 formation rate/(mmol·gCo−1·min−1) Ref. 14.7 ± 0.2 Co15@MC 400 36000 100 — [21] 14.7 ± 0.1 Co15@AC 400 36000 100 — [21] — 90CoAl 600 18000 ~ 100 — [22] 5 Co/MWCNTs 500 6000 25 4.0 [23] 5 Co/CeO2-3DOM 500 6000 62 4.2 [24] 5 5CoTi-NT 550 6000 19 0.41 [25] 10 10CoNaTi-NT 500 6000 ~ 18 0.35 [25] — Co/SiO2 500 30000 13 4.3 [26] 4.8 Co-BaNH 500 36000 — 20.0 [27] 7 Co/Ax-21 500 5200 ~ 60 — [28] 7.7 Co/Al2O3-precipitation 500 22000 ~ 55 156.4 [29] 5 Co/MgO-La2O3 500 6000 60 4 [30] 18.7 CoOx@C-700-A 500 15000 ~ 55 8.8 [31] — CoX (X = Mn, Cr) 500 24000 35 9.4 [32] 5 5CMLa-2 500 6000 8 0.5 [33]
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表 3 Ni基催化剂氨分解活性对比
Table 3. The comparison of catalytic activity over Ni based catalysts for NH3 decomposition
Ni loading/wt% Catalyst T/°C GHSV/(mL·gcat−1·h−1) NH3 conv./% H2 formation rate/(mmol·gNi−1·min−1) Ref. 5 Ni/rGO 700 — 81.9 27.4 [34] 5 Ni/carbon xerogel 600 13000 100 — [35] 11.1 Ni/graphene aerogel 600 30000 70.2 21.6 [36] 38.6 Ni-50/APT 650 30000 89.9 30.1 [37] 8.7 Ni-30/ATP@SiO2 650 30000 73.4 24.6 [37] — Ni/CaNH 500 15000 71 11.8 [38] — Ni/CaNH-HS 500 15000 91 15.3 [38] 5 Ni/ZSM-5 650 6000 100 — [39] 23.4 Ni/SBA-15 550 30000 87 24.9 [40] 10 Ni/Y2O3 550 0.6* ~ 88 — [41] 30 Ni/Al2O3 550 — 68 — [42] 30 Ni/Y2O3 550 — 98 — [42] 30 Ni/CeO2 550 — 93 — [42] 30 Ni/MgO 550 — 87 — [42] 30 Ni/La2O3 550 — 84 — [42] 30 Ni/ZrO2 550 — 72 — [42] — Ni/CeO2-BN 600 30000 77 25.8 [43] 20 La-Ni/Al2O3 550 6000 92 — [44] 20 Ba-Ni/Al2O3 550 6000 95 — [44] — Ce10-NiO-SiO2-350 650 3000 mL/h 99 33.24 [45] * weight/flow (W/F)
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表 4 多组分金属催化剂氨分解活性对比
Table 4. The comparison of catalytic activity over multi-component-based catalysts for NH3 decomposition
Metal loading/wt% Catalyst T/°C GHSV/(mL·gcat−1·h−1) NH3 conv./% H2 formation rate/(mmol·gcat−1·min−1) Ref. — Rh-Pt 550 16000 (1%NH3) 100 — [75] 0.97 Ru-Fe-C 600 20.0 97.5 21.7 [76] 2.5Ni-0.5Ru Ni-Ru/CeO2 450 — ~ 99 — [67] — Ru-Co@N-C 700 12000 ~ 97 — [77] — Cu-Zn/Al2O3 500 0.7* ~ 95 0.7 [78] 10 6Fe-4Ni 500 14400 28 — [60] 10 Ni5Co5/fumed SiO2 550 30000 76.8 25.7 [63] 5Co-5Ni Co-Ni/Al2O3 650 30000 90.0 — [61] 5Fe-5Ni Fe-Ni/Al2O3 650 30000 ~ 12 — [61] 5Cu-5Ni Cu-Ni/Al2O3 650 30000 ~ 22 — [61] 5Fe-5Mo Fe5Mo5/YSZ 600 46000 50 — [79] 8.3Fe-1.7Ni Fe-Ni/Al2O3 650 28500 99.8 — [62] — Fused Fe-Co 600 24000 ~ 40 — [57] — Co0.89FeO2.11@mSiO2 600 60000 ~ 88 8 [59] 5 CoFe5-in-CNTs 600 36000 48 — [12] 5 CoMo/Al2O3 600 36000 99.5 8 [68] 5 CoMo/MCM-41 600 36000 99 26 [69] bulk 3CoMoN 600 6000 98.3 — [71] — CoMoNx/CNT 550 11000 84.4 — [72] 1%Ni, 9%Co Ni1Co9/CZY 350 6000 ~ 12 0.71 [64] 13.2 4Ni/Ce0.8Zr0.2
O2-SA550 — 97 3.99 [80] 1.2%Ni, 0.1%Ce Ni1.2Ce0.1/Al2O3 600 30000 71.9 24.1 [80] 1.0%−5.0%Ni,
< 1%PtNi-Pt/Al2O3 600 6600 78.1 — [81] 2.5Ni-0.5Ru Ni-Ru/CeO2 450 — ~ 99 — [67] 10Ni-0.7Ir Ni-Ir/γ-Al2O3 400 9500 43.6 — [82] 4.1%Ni, 6.7%Mo NiMoNy/α-Al2O3 600 3600 78.9 — [83] 68.1La2O3-29.6CeO2 La2O3-CeO2 250 — 100 — [84] 9.3 HEA-Co55Mo15 500 36000 100 — [73] 60 K-CoNialloy-MgO-CeO2-SrO 500 12000 100 57.75 [65] *mmol/(gcat·min)
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表 5 等离子体辅助过渡金属基催化剂氨分解活性对比
Table 5. Comparison of ammonia decomposition activity of plasma-assisted transition metal-based catalysts
Metal loading/wt% Catalyst T/°C GHSV/(mL·gcat−1·h−1) NH3 conv./% H2 formation rate/(mmol·gcat−1·min−1) Ref. 94.4%FeO FeO 410 — 100 — [87] 10 Fe/SiO2 450 — 71.7 2.2 [88] 10 Ni/SiO2 450 — 86.3 2.7 [88] 10 Co/SiO2 450 — 99.2 3 [88] 10 6Fe-4Ni 500 14400 99.9 16 [60] 10 9Fe-1Ni 460 14400 49.4 8 [60] 10 7Fe-3Ni 460 14400 55.0 8.8 [60] 10 5Fe-5Ni 460 14400 59.6 9.5 [60] 10 2Fe-8Ni 460 14400 46.0 7.3 [60] 5 FeCo/CeO2-S 500 36000 73 29.3 [58] 5 FeNi/CeO2-S 500 36000 64 25.7 [58] 5 CoNi/CeO2-S 500 36000 51 20.5 [58] 30 Co/fumed SiO2 450 — ~ 97 — [89] ammol/(gcat·h)
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