Emerging trends in research and development on earth abundant materials for ammonia degradation coupled with H₂ generation

Figures & data

Figure 1. (a) Energy density of a range of chemical fuels. (b) Estimated rise in annual ammonia production.

Table 1. Fuel-associated ammonia technologies.

S. No.	Efficiency	Required pre-treatment	Per capita cost* (in $/kW)
1.	Proton exchange membrane fuel cell	i) Decomposition of ammonia	100 (mobile)
		ii) Trace content of ammonia removal	1300 (static)
2.	Alkaline fuel cell	None	1300 (static)
3.	Solid oxide fuel cell	None	760 (static)
4.	Internal combustion engine	Partial decomposition of ammonia	30–45 (mobile)
			1000 (static)
5.	Boilers and furnaces	None	150–350 (static)
6.	Combined cycle gas turbines	Partial decomposition of ammonia	750 (static)

*Estimated cost for both mobile and static applications are based on recently developed technologies.

Figure 2. Estimated net zero carbon energy goals from 2020 till the end of the year 2050 (citation: 2020, International Energy Agency (IEA)).

Figure 3. Various hydrogen production pathways.

Table 2. Summary of the basic conditions for H₂ production through non-renewable sources.

Process	Raw material/ feed stock	Chemical-equation followed	Temperature required (ºC)	By-product	Nature
Steam reforming	Lighter hydro-carbons (LPG or coal)	$\mathrm{C}{\mathrm{H}}_4+H_2\mathrm{O}\to \mathit{C}{O}_2\mathit{\hspace{0.17em}}+{\mathrm{H}}_2$	800–1000	CO, CO2	Endothermic
Partial methane oxidation	Methane, Heavy fuel oil	$\mathrm{C}{\mathrm{H}}_4+1/2O_2\to \mathit{CO}\mathit{\hspace{0.17em}}+2{\mathrm{H}}_2$	>1000	CO, CO2	Exothermic
Coal gasification	Coal	$\mathrm{C}\left(\mathrm{coal}\right)+O_2+H_2\mathrm{O}\to \mathit{C}{O}_2\mathit{\hspace{0.17em}}+{\mathrm{H}}_2$	700–1800	CO, CO2	Exothermic
Pyrolysis	Hydrocarbons	$C_X{H}_{\mathit{Y}}\to \mathit{xC}+\frac{1}{2}\mathit{y}{H}_2$ $C_X{H}_{\mathit{Y}}+\left(2\mathit{x}-\frac{y}{2}\right)H_2\to \mathit{xC}{H}_4$ $\mathit{C}{H}_4\to \mathit{C}+2H_2$	500–800	C (solid), CH4	Endothermic
Biomass derived liquid reforming	Methanol, Ethanol, Sugars, Acetic acid	$C_2{H}_5\mathit{OH}+H_2\mathrm{O}\to \mathit{C}{O}_2\mathit{\hspace{0.17em}}+{\mathrm{H}}_2$ $\mathrm{C}{\mathrm{H}}_3\mathrm{OH}+H_2\mathrm{O}\to \mathit{C}{O}_2\mathit{\hspace{0.17em}}+{\mathrm{H}}_2$	>800	CO, CO2	Endothermic

LPG: Liquefied Petroleum Gas.

Table 3. Different hydrogen production technologies from a renewable source of water.

Technology	Source	Temperature required (ºC)	By-product
Electrolysis	Electricity	40–900	O2
Photo electrolysis	Light/solar energy	>1200	O2
Thermolysis	Heat	>2500	O2
Bio-photolysis	Microbes	Ambient conditions	O2

Figure 4. Catalytic activity for ammonia decomposition over alkaline earth metals modified Ni/Y₂O₃; (a) TEM images, (b) particle size distribution, (c) NH₃ conversion percentage, and (d) stability performance of SrO-Ni/Y₂O₃ (5:40 wt%), (copyright @ 2016 RSC Advances).

Figure 5. Incorporation of catalytic membrane for ADR process. (a) Schematic catalytic membrane reactor, (b) catalytic activities, (c) TEM image of bimodal, (d) TEM image of monomodal, and e) SEM image of bimodal catalytic membrane (copyright @ 2011 Elsevier). (f) Mechanistic interaction of Ru doping in La_xCe_1-xO_y composites and (g) catalytic performance by varying different temperature for NH₃ conversion (copyright @ 2021 Elsevier).

Table 4. Catalysts based on noble metals utilization to decompose ammonia.

Active phase	Supported on	% NH3 conversion	References
Ru	@La2O3−ZrO2	34	[63]
Ru	@La2O3−ZrO2	81	[64]
Ru	@SiO2	63	[64]
Ru	@SiO2	96	[63]
Ru	[Ca24Al28O64]^4+(O^2−)2	73	[65]
Ru	[Ca24Al28O64]^4+(e−)4	42	[53]
Ru	AC	70	[53]
Ru	AC	25	[66]
Ru	AC	4	[67]
Ru	AC	5	[68]
Ru	Al2O3	7	[69]
Ru	Al2O3	13	[53]
Ru	Al2O3	37	[70]
Ru	Al2O3	7	[54]
Ru	MgO	39	[71]
Ru	MgO	29	[72]
Ru	MgO	76	[73]
Ru	MgO-Al2O3	86	[74]
Ru	MgO-MIL-101	45	[75]
Ru	MgO-MIL-101	88	[75]
Ru	MgyAlzOn	17	[76]
Ru	MIL-101	42	[75]
Ru	MIL-101	66	[75]
Ru	MWCNT	31	[71]
Ru	Na2Ti3O7	86	[77]
Ru	N-CNTs	48	[78]
Ru	N-CNTs	85	[77]
Ru	N-OMC	69	[78]
Ru	O-CNFs	59	[55]
Ru	OMC	41	[55]
Ru	Pr6O11	20	[55]
Ru	Pr6O11	19	[55]
Ru	Pr6O11	49	[55]
Ru	Pr6O11	27	[55]
Ir	Al2O3	86	[79]
Ir	Al2O3	45	[80]
Ir	SiO2	88	[80]
Pd	SiO2	17	[81]
Pd	Al2O3	42	[79]
Pd	SiO2	31	[81]
Pt	Al2O3	86	[79]
Pt	Al2O3	61	[62]
Pt	MCM- 41	85	[82]
Pt	SiO2	69	[82]
Rh	Nb2O5	20	[61]
Rh	SiO2	19	[61]

Figure 6. Varying different temperature for NH₃ conversion over iron-based nanostructured composites (a) 1st catalytic performance, (b) 2nd catalytic performance, and (c) stability performance (copyright @ 2015 Elsevier). Varying different temperature for NH₃ conversion over ceria-based oxide supported nickel composites (d) catalytic performance, (e) Arrhenius plot, and (f) stability performance (copyright @ 2020 Elsevier). (g) Varying different temperature for NH₃ conversion over ceria-based oxide supported Ni, Ru, and Ni-Ru composites (copyright @ 2019 Elsevier), varying different temperature for NH₃ conversion over ceria-based oxide supported Ru/Al₂O₃ composites. (h) Comparative study with literature reports and (i) catalytic performance (copyright @ 2023 Elsevier).

Figure 7. NH₃ decomposition by (a) ion exchange method, (b) NaOH deposition method, (c) TEM images of 1. 10CoTi-NT 2. 10CoNaTi-NT (copyright @ 2019 Elsevier). (d) Synthesis scheme of MoS₂ catalysts, (e) catalytic activity of MoS₂ composites, and (f) stability performance (copyright @ 2020 Elsevier).

Table 5. Efficiency of reported non-noble metal catalysts for ammonia-decomposition.

Active phase	Supported on	% NH3 flow	% NH3 conversion	References
Ni	@SiO2	100	36	[63]
Ni	@SiO2	100	40	[63]
Ni	@SiO2	100	87	[109]
Ni	@SiO2	100	47	[63]
Ni	AC	0.2	2	[110]
Ni	AC	15	75	[111]
Ni	Al2O3	100	15	[85]
Ni	Al2O3	100	15	[112]
Ni	Al2O3	100	17	[113]
Ni	Al2O3	100	97	[114]
Ni	Al2O3	100	33	[115]
Ni	Al2O3	100	27	[89]
Ni	Al-Ce0.8Zr0.2O2	100	58	[94]
Ni	attapulgite	100	90	[116]
Fe	@ Al2O3	100	9	[117]
Fe	@CeO2	100	70	[92]
Fe	@SiO2	100	8	[91]
Fe	@SiO2	100	17	[91]
Fe	@SiO2-Cs	100	16	[91]
Fe	@TiO2	100	60	[92]
Fe	AC	0.2	90	[111]
Fe	Al2O3	100	–	[79]
Fe	Al2O3	50	25	[118]
Fe	Al2O3	100	86	[83]
Fe	C/SBA-15	100	32	[113]
Fe	Carbon	0.2	96	[119]
Fe	CMK-5	100	74	[113]
Fe	CNFs	100	51	[120]
Co	AC	100	34	[121]
Co	AC	100	2	[122]
Co	Al2O3	100	–	[79]
Co	Al2O3	100	21	[123]
Co	Al2O3	100	100	[83]
Co	Al2O3	100	44	[124]
Co	Al2O3	100	57	[98]
Co	AX-21	100	25	[125]
Co	AX-21	100	3	[125]
Co	Ce0.6Zr0.3Y0.1O2	100	7	[126]
Co	CeO2	100	30	[126]
Co	CNTs	100	100	[127]
Co	CNTs	100	61	[128]
Co	CNTs	100	–	[129]
Co	CNTs	100	–	[130]
Co	CNTs	100	8	[131]
Co	CNTs	100	9	[122]
Mo	Al2O3	100	22	[123]
Mo	C	100	66	[108]
Mo	MCM-41	100	28	[132]
Mo	Y2O3-ZrO2	100	10	[133]
MoN	C	100	82	[108]
MoN	SBA-15	100	69	[134]
MoN	SiO2	100	50	[134]
MoN	Al2O3	100	99	[135]
MoS2	Al-laponite	10	46	[106]
MoS2	Laponite	10	35	[106]
MoS2	Ti-laponite	10	74	[106]
MoS2	Zr-laponite	10	94	[106]
Mo2C	–	100	–	[136]
Mo2C	–	100	77	[107]
Mo2N	–	100	94	[137]
Mo2N	–	100	10	[138]
Mo2N	–	100	100	[139]

Table 6. Catalytic activity of metallic amides, imides, carbides, and nitrides.

Active phase	% NH3 inlet flow	% NH3 conversion	References
CrN	100	0	[130]
Fe2N	100	4	[147]
Fe2N	100	–	[130]
Fe3C	100	23	[148]
MnN	5	15	[149]
WC	100	22	[137]
V8C7	100	–	[136]
K2[Mn(NH2)4]	5	48	[149]
Li2Ca(NH)2	100	48	[142]
Li2Mg(NH)2	100	40	[142]
Li2NH	5	0	[73]
Li2NH	100	26	[130]
Li2NH-Co	–	–	[130]
Ru-KNH2	10	96	[140]
Ru-LiNH2	5	100	[73]
Ru-Mg(NH2)2	100	3	[150]
Ru-NaNH2	10	97	[140]

Figure 8. Ammonia decomposition over bimetallic Ni- and Co-based catalyst (copyright @ 2019 Elsevier).

Figure 9. Schematic illustration of PEM fuel cell for H₂ production from ammonia (copyright @ 2018 Elsevier).

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