氨氧化技术在清洁能源开发和污水净化中的研究进展

doi:10.1016/S1872-2067(23)64537-1

催化学报 ›› 2023, Vol. 54: 161-177.DOI: 10.1016/S1872-2067(23)64537-1

氨氧化技术在清洁能源开发和污水净化中的研究进展

张颖贞^a, 黄剑莹^a^,^b^,^*(), 赖跃坤^a^,^b^,^*()

^a福州大学石油化工学院, 国家化肥催化剂工程研究中心, 福建福州350116
^b清源创新实验室, 福建泉州362801

收稿日期:2023-06-12 接受日期:2023-09-27 出版日期:2023-11-18 发布日期:2023-11-15
通讯作者: *电子信箱: yklai@fzu.edu.cn (赖跃坤), jyhuang@fzu.edu.cn (黄剑莹).
基金资助:
国家自然科学基金(22075046);国家自然科学基金(51972063);国家重点研发计划(2022YFB3804905);国家重点研发计划(2022YFB3804900);国家重点研发计划(2019YFE0111200);福建省杰出青年自然科学基金(2020J06038);福建省杰出青年自然科学基金(2019J01256);111工程(D17005)

Recent advances of ammoxidation in clean energy exploitation and sewage purification: A mini review

Yingzhen Zhang^a, Jianying Huang^a^,^b^,^*(), Yuekun Lai^a^,^b^,^*()

^aNational Engineering Research Center of Chemical Fertilizer Catalyst (NERC-CFC), College of Chemical Engineering, Fuzhou University, Fuzhou 350116, Fujian, China
^bQingyuan Innovation Laboratory, Quanzhou 362801, Fujian, China

Received:2023-06-12 Accepted:2023-09-27 Online:2023-11-18 Published:2023-11-15
Contact: *E-mail: yklai@fzu.edu.cn (Y. Lai), jyhuang@fzu.edu.cn (J. Huang).
About author:Jianying Huang received PhD degree in 2007 from College of Chemistry and Chemical Engineering, Xiamen University. During 2007-2011, she is an assistant professor at Fujian Institute of Research on the Structure of Matter. Later, she acted as visiting scholar at Muenster University. From 2013 to 2018, she was an associate professor at School of Textile and Clothing Engineering in Soochow University. Currently, she is a full professor at College of Chemical Engineering at Fuzhou University, and selected as the 2019-2022 Highly Cited Researchers. Her research interests focus on bio-inspired surfaces with special wettability, advanced materials for energy and environmental applications.
Yuekun Lai is a Fujian province “Minjiang Scholar” Chair Professor at the College of Chemical Engineering at Fuzhou University, and served as Editor of Chemical Engineering Journal. He received his PhD degree from the Department of Chemistry, Xiamen University. He is selected as the 2018-2022 Highly Cited Researchers (Clarivate Analytics) and the recipient of the 2016 Journal of Materials Chemistry A (JMCA, RSC) Emerging Investigators and 2019 Advanced Materials Interfaces (AMI, Wiley) Hall of Fame award. His current research topics are bioinspired intelligent materials with special wettability, multifunctional fabrics, conductive hydrogels and functional nanostructures for energy and environmental applications.
Supported by:
National Natural Science Foundation of China(22075046);National Natural Science Foundation of China(51972063);National Key Research and Development Program of China(2022YFB3804905);National Key Research and Development Program of China(2022YFB3804900);National Key Research and Development Program of China(2019YFE0111200);Natural Science Funds for Distinguished Young Scholar of Fujian Province(2020J06038);Natural Science Foundation of Fujian Province(2019J01256);111 Project(D17005)

摘要/Abstract

摘要：

随着经济的发展, 当今社会对能源的需求不断增加. 然而, 传统的化石燃料, 如煤和石油, 虽然能够提供大量的能源, 但其资源有限, 不可再生, 并且燃烧产物对环境有害, 不符合绿色低碳的发展理念, 亟需开发新型、高效的清洁能源. 氨(NH₃)因具有氢含量高、燃烧产物(完全燃烧时产物为N₂和H₂O)无害、可规模化生产、压缩性好、易于储存和运输等优点, 被认为是直接氨燃料电池(DAFCs)的理想候选燃料. 同时, 氨也是常见的含氮污染物, 广泛存在于人类生产和工农业活动中. 因此, 氨氧化反应(AOR)在清洁能源生产和含氨废水处理领域都起着重要作用.

本文首先系统总结了AOR在不同领域的研究进展, 强调了其在清洁能源领域(如DAFCs)的巨大应用潜力, 突出了AOR与水电解反应中的阴极氢析出过程耦合制取氢气在能源转化领域的研究价值, 以及AOR在含氨废水处理领域的重要性. 然后, 讨论了AOR机制: AOR反应过程中存在竞争, 并可生成多种含氮产物(如N₂, NO, NO₂, NO₂^-和NO₃^-等), 进而影响产物的选择性和反应效率等. 再后, 讨论了原位表征技术(如采用原位拉曼光谱对催化剂重构行为跟踪和采用原位傅里叶变换红外光谱对反应中间体实时监测)和构建理论计算模型的重要性, 这些方法为揭示AOR机制和反应路径提供有力的支持. 同时, 对AOR催化剂的设计策略和反应条件的筛选提出建议, 如反应环境pH值会影响活性位点的质子化状态, 从而改变吸附行为, 影响催化性能. 还探讨了AOR过程耦合电解水氢析反应对低能耗、高效率制取氢气的意义, 并概述了在含氨废水处理中提高氮气产物选择性的必要性. 最后, 讨论了AOR研究中面临的挑战和可采用的策略, 包括进一步增加活性位点的暴露、增强催化活性、精准识别活性位点、最大程度地利用催化中心、提高催化剂抗中毒能力、提高目标产物的选择性以及提高催化剂使用寿命等.

综上, 本文系统地总结了AOR的研究进展、反应机制以及未来的发展策略等, 为进一步推动AOR在洁净能源和环境保护领域的应用, 为进一步开发更绿色环保的能源体系以及高效的污水处理方法提供新思路.

关键词: 氨氧化反应, 直接氨燃料电池, 氢气, 污水处理, 清洁能源, 电催化

Abstract:

In recent decades, the advancement of clean energy technologies and sewage purification has emerged as a focal point of research. This review focuses on the ammonia oxidation reaction (AOR) and summarizes its multifaceted applications, including its use in direct ammonia fuel cells (DAFCs), its coupling with the hydrogen evolution reaction (HER), and its significance in ammonia-containing sewage purification. We discuss how the combination of in-situ characterization techniques and theoretical models has emerged as a powerful tool for exploring the AOR mechanism. The interplay of operational parameters such as temperature and pH, along with catalyst design, is emphasized in the context of DAFCs, highlighting the need for precise optimization to enhance efficiency. The importance of selectivity in the nitrogen gas product in ammonia-containing wastewater is also discussed. Furthermore, the review addresses the challenges and opportunities in AOR research, including strategies to enhance catalytic activity, identify active centers, maximize the utilization of catalyst atoms, and improve selectivity while ensuring catalyst durability. Ultimately, this review serves as a comprehensive guide for researchers and practitioners interested in harnessing the potential of AOR to bridge the gap between clean energy generation and sustainable wastewater treatment, offering insights into a greener and more environmentally responsible future.

Key words: Ammonia oxidation reaction, Direct ammonia fuel cells, Hydrogen, Sewage purification, Clean energy, Electrocatalysis

张颖贞, 黄剑莹, 赖跃坤. 氨氧化技术在清洁能源开发和污水净化中的研究进展[J]. 催化学报, 2023, 54: 161-177.

Yingzhen Zhang, Jianying Huang, Yuekun Lai. Recent advances of ammoxidation in clean energy exploitation and sewage purification: A mini review[J]. Chinese Journal of Catalysis, 2023, 54: 161-177.

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图/表 16

Fig. 1. (a) Comparison of volumetric energy densities of different energy sources. Reprinted with permission from Ref. [5]. Copyright 2022, Elsevier. (b) Schematic of a DAFC. Reprinted with permission from Ref. [19]. Copyright 2022, Elsevier. (c) Diagram of AOR coupled with HER. (d) The pathways of AOR in acidic (pH = 0) and basic (pH = 14) conditions. Reprinted with permission from Ref. [17]. Copyright 2023, American Chemical Society.

Fig. 2. The typical development process and future challenges of AOR. Reprinted with permission from Ref. [33]. Copyright 2021, John Wiley and Sons. Reprinted with permission from Ref. [34]. Copyright 2023, Springer Nature.

Fig. 3. Diagram of AOR and the production of N2, NO2- and NO3- byproducts according to the O-S mechanism (green) and G-M mechanism (blue).

Fig. 4. (a) Estimated AOR onset potential for close-packed facets of transition metals. The colors indicate the determining steps for each metal. (b) Activity as predicted by Sabatier analysis for both mechanisms at 0 V vs. RHE. Reprinted with permission from Ref. [36]. Copyright 2015, American Chemical Society. Free energy diagram of AOR on Pt(111) (c) and Cu(111) (d) at 0 V vs. RHE. All energies are given with adsorbates at infinite separation, 1/9 ML coverage. Zero energy corresponds to N2 (g). Reprinted with permission from Ref. [36]. Copyright 2015, American Chemical Society.

Fig. 5. (a) Adsorption energy of different AOR intermediates on Pt3-xIrx. Reprinted with permission from Ref. [37]. Copyright 2018, Elsevier. (b) AOR reaction diagram on PtIrNi/SiO2-CNT-COOH. Gibbs free energy (c), corresponding reaction models (d), and d-orbital densities (e) on Pt(100), Pt3Ir(100) and Pt3IrNi(100). Reprinted with permission from Ref. [38]. Copyright 2020, American Chemical Society. (f) Possible products of AOR. (g) Binding energies of the reactants, intermediates, and products on different metals. Reprinted with permission from Ref. [39]. Copyright 2022, Royal Society of Chemistry.

Fig. 6. (a) Binding energies of Fe7, Fe7Ni, Fe7Mo, and Fe7Co clusters, from left to right. (b) Electron cloud density of NH3 and Fe7, Fe6Ni(l and t), Fe6Mo(l and t), and Fe6Co(l and t)clusters. (c) Relationship between d-band center and ammonia adsorption energy. (d) Gibbs energy free and (e) intermediates geometries of NH3 on Fe6Mo(t). Reprinted with permission from Ref. [40]. Copyright 2022, Elsevier.

Fig. 7. (a) In-situ FTIR spectra of AOR on Pt surface at different potentials. (b) Potential dependence of AOR current density at the Pt electrode and the intensity of corresponding FTIR spectra. (c) AOR pathways on Pt surface. Reprinted with permission from Ref. [46]. Copyright 2015, American Chemical Society.

Fig. 8. (a) In-situ UV-Vis spectra of AgNPs and Agn0 during thermal catalysis. (b,c) In-situ FTIR spectra of the AOR process performed at different temperatures. (d) Selectivity of AOR. Reprinted with permission from Ref. [47]. Copyright 2021, American Chemical Society.

Fig. 9. (a,b) Cyclic voltammetry (CV) and power density curves of DAFC in KOH solutions with various concentrations. Reprinted with permission from Ref. [22]. Copyright 2019, Elsevier. CV curves (c), electrochemical impedance spectroscopy (EIS) data (d), and AOR activity (e) of PtIrZn2/CeO2-ZIF-8 at various KOH concentrations. (f) Electrochemical performance curves of DAFCs with PtIrZn2/SiO2-CNT-COOH and other contrast electrodes. Reprinted with permission from Ref. [49]. Copyright 2021, RSC Publishing. (g) CV curves and (h) Ea of NiCu@NiCuOOH and NiCu, in 2.0 mol L-1 NaOH containing 0.4 mol L-1 NH4Cl. (i) Electrochemical performance curves in different concentrations of NaOH with 0.4 mol L-1 NH4Cl. Reprinted with permission from Ref. [50]. Copyright 2022, Elsevier.

Fig. 10. (a) Electrochemical performance curves of PtRu/C as anode and Pd/C as cathode, under 25, 40, 60, 80, and 95 °C, respectively. Reprinted with permission from Ref. [51]. Copyright 2022, American Chemical Society. (b) PtIr as anode and LaCr0.25Fe0.25Co0.5O3-δ (LCFCO) as cathode, at 20, 40, 60, 80, and 100 °C, respectively. (c) PtIr as anode, and LCFCO as cathode, compared with Pt/C as cathode, at 70 and 80 °C, respectively. Reprinted with permission from Ref. [52]. Copyright 2022, Elsevier. (d) CV curves of PtIr/C catalyst in 1.0 mol L-1 KOH saturated with Ar-NH3 vapor, recorded at a scan rate of 20 mV s-1, and 25, 40, 50, and 60 °C, respectively. Reprinted with permission from Ref. [53]. Copyright 2018, The Electrochemical Society.

Fig. 11. Preparation process diagram of the PtPb nanocatalysts (a), their particle size distribution (b), and TEM image (c). (d) CV curves of PtPb/C in 1.0 mol L-1 KOH with or without 0.1 mol L-1 NH3·H2O recorded at a scan rate of 10 mV s-1. (e) CV curves of PtPb/C in 1.0 mol L-1 KOH with 0.1 mol L-1 NH3·H2O. (f) Chronopotentiometry curves of PtPb/C and Pt/C at 50 mA mg-1Pt. Reprinted with permission from Ref. [71]. Copyright 2023, American Chemical Society.

Fig. 12. CV curves of Ni/MnO2 (a), Cu/MnO2 (b), and NiCu/MnO2 (c) in 0.5 mol L-1 NaOH with or without 55 mmol L-1 NH4Cl. (d) CA (chronoampetometry) curves for Ni/MnO2, Cu/MnO2, and NiCu/MnO2 at +0.6 V vs. Hg/HgO. (e) Faradic efficiencies obtained with NiCu/MnO2 at a constant potential from +0.6 to +1.0 V in a 0.5 mol L-1 NaOH electrolyte containing 55 mmol L-1 NH4Cl. Reprinted with permission from Ref. [79]. Copyright 2021, American Chemical Society. (f) The energy barriers of the different reaction steps in Ni-Cu-Fe-OOH and Ni-Cu-OOH, inset demonstrates the energy barriers for the divergence steps of the G-M mechanism and the O-S mechanism in the Ni-Cu-Fe-OOH system. (g) CV curves of a-NiCuFe and a-NiCu in 0.5 mol L-1 NaOH with or without 55 mmol L-1 NH4Cl. (h) Time-dependent UV-Vis spectra of an NH3-containing solution tested for AOR. (i) NH3 removal efficiency and Faradaic efficiency of a-NiCuFe at different applied potentials. Reprinted with permission from Ref. [81]. Copyright 2021, John Wiley and Sons.

Fig. 13. (a) The time-dependent concentration profiles of NH4+, NO2-, and NO3- over time, at an applied current density of 30 mA cm-2. (b) XPS spectra of NiO-TiO2 before and after reaction, indicating changes in the material's composition and surface chemistry. Reprinted with permission from Ref. [27]. Copyright 2020, Elsevier. (c,d) The correlation between pH values and the effect of pH on nitrate generation of N2 and NO3- at C0(NH3) 10 mg L-1. Reprinted with permission from Ref. [82]. Copyright 2021, Elsevier. (e) Removal efficiency and selectivity on PtCu/G electrodes by different applied current density (CD) and C0 of NH3. (f) Reaction diagram of AOR on metal oxides. Reprinted with permission from Ref. [26]. Copyright 2022, American Chemical Society.

Fig. 14. Free energy diagrams for the conversion of NH3 to NO3-, via the O-S mechanism (a) and the G-M mechanism (b). (c) Representation of the lowest energy configurations for AOR intermediates. Reprinted with permission from Ref. [86]. Copyright 2021, John Wiley and Sons.

Table 1 Comparative analysis of AOR performance among Ni-based, Cu-based, and other metal catalysts.

Material	Preparation	Electrolyte	Method	j (mA cm^-2)	Field	Ref.
Ni(OH)₂	sol-gel method	0.1 mol L^-1 NaOH + 0.2 mol L^-1 NH₃	EC	70	Purify Sewage	[25]
NiO/TiO₂	solution combustion	0.1 mol L^-1 NaNO₃ + 0.2 mol L^-1 NH₄OH	EC	2	Purify Sewage	[27]
MgO/Co₃O₄	Co-precipitation	1.0 mol L^-1 NaOH + 30 ppm NH₄Cl	COA	NA	Purify Sewage	[28]
PtIrNi₁/SiO₂-CNT-COOH	sonochemical-assistance	1.0 mol L^-1 KOH + 0.1 mol L^-1 NH₃	EC	120 A g^-1	AOR	[38]
PtIrZn/CeO₂-ZIF-8	sonochemical-assistance	1.0 mol L^-1 KOH + 0.1 mol L^-1 NH₃	EC	44 A g^-1	DAFC	[49]
NiCu@NiCuOOH	electrooxidation	2.0 mol L^-1 NaOH + 0.4 mol L^-1 NH₄Cl	EC	100	DAFC	[50]
PtRu/C	commercial	3.0 mol L^-1 KOH + 3.0 mol L^-1 NH₃	EC	NA	DAFC	[51]
LaCr_0.25Fe_0.25Co_0.5O_3-_δ	physically mix	1.0 mol L^-1 KOH + 7.0 mol L^-1 NH₃	EC	NA	DAFC	[52]
PtPb/C	solvothermal	1.0 mol L^-1 KOH + 0.1 mol L^-1 NH₃	EC	191.2	AOR-H₂	[71]
TiO/Ti foil	calcined	0.5 mol L^-1 NaOH + 0.1 mol L^-1 NH₃	EC	0.06	AOR-H₂ or DAFC	[72]
Ni₂P/NF	hydrothermal and annealed	0.1 mol L^-1 KOH + 1000 ppm NH₃	EC	13	Purify Sewage	[74]
Ni₁Cu₃-S-T/CP	hydrothermal and annealed	1.0 mol L^-1 NaOH + 0.2 mol L^-1 NH₄Cl	EC	130	Purify Sewage	[78]
NiCu/MnO₂	electrodeposition	0.5 mol L^-1 NaOH + 55 mmol L^-1 NH₄Cl	EC	30	Purify Sewage	[79]
NiCuFe	electrodeposition	0.5 mol L^-1 NaOH + 55 mmol L^-1 NH₄Cl	EC	60	Purify Sewage	[81]
NiCu/CP	electrodeposition	0.5 mol L^-1 NaOH + 55 mmol L^-1 NH₄Cl	EC	52	AOR	[93]
Ni(OH)₂/SnO₂	hydrothermal and annealed	0.5 mol L^-1 K₂SO₄ + 10 mmol L^-1 NH₃	EC	4.5	Purify Sewage	[94]
Au@Pt NPs	seed-mediated growth method	1.0 mol L^-1 NaOH + 0.05 mol L^-1 NH₃	PEC	1.1	AOR	[95]
FePi/Fe₂O₃	hydrothermal and annealed	0.1 mol L^-1 NaOH + 500 ppm NH₃	PEC	1.2	Purify sewage	[96]
SL C₃N₄	annealed	1.5 mg L^-1 NH₃	PC	NA	Purify sewage	[97]

Fig. 15. Exploring catalyst design ideas, real-time catalyst monitoring in electrochemical processes, innovative approaches for detecting AOR reaction intermediates, and the multidisciplinary research significance of AOR across various fields.

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氨氧化技术在清洁能源开发和污水净化中的研究进展

Recent advances of ammoxidation in clean energy exploitation and sewage purification: A mini review

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