Unveiling the Au-Mn-Cu synergy in Au/LaMnCuO3 catalysts for selective ethanol oxidation

doi:10.1016/S1872-2067(25)64686-9

Abstract

Abstract:

Gold nanoparticles (AuNPs) supported on the Cu-doped LaMnO₃ perovskites exhibit strong Au-Mn-Cu synergy in the aerobic oxidation of gaseous ethanol to acetaldehyde (AC). The Au/LaMnCuO₃ catalysts achieve AC yields exceeding 90% and a space-time yield of 715 g_AC g_Au^-1 h^-1 at 225 °C, outperforming reported catalysts. The outstanding performance is attributed to adjacent Cu⁺ and Mn²⁺ ions in the perovskite surface, which, together with nearby AuNPs, contribute to the high activity and stability. The best-performing catalyst contains a Cu/Mn ratio of 1/3 in the perovskite. Doping too much Cu into the perovskite leads to metallic Cu, suppressing catalyst performance. Density functional theory (reaction energetics, electronic structure analysis) and microkinetics simulations aided in understanding the synergy between Cu and Mn and the role of AuNPs. The reaction involves two H abstraction steps: (1) O-H cleavage of adsorbed ethanol by the basic perovskite lattice oxygen atom and (2) α-C-H cleavage by AuNPs, yielding AC and adsorbed water. Molecular O₂ adsorbs in the oxygen vacancy (O_V) formed by water removal, generating a peroxide anion (O₂^2-) as the activated oxygen species. In the second part of the catalytic cycle, the basic O₂^2- species abstracts the H atom from another ethanol molecule, followed by α-C-H cleavage by AuNPs, AC production, and water removal. Water formation in the second part of the catalytic cycle is the rate-controlling step for Au/LaMnO₃ and Au/LaMnCuO₃ models. Moderate Cu doping enhances the essential Cu⁺-O_V-Mn²⁺ sites and lowers the barrier for water formation due to the weaker Cu-O bond than the Mn-O bond. In contrast, excessive Cu doping creates unstable Cu²⁺-O-Cu²⁺ sites and shifts the barrier to the α-C-H cleavage.

Key words: Ethanol oxidation, Acetaldehyde, Gold catalyst, LaMnO₃ perovskite, Copper doping

Wang Jie, Chen Lulu, Yue Lijun, A. W. Filot Ivo, J. M. Hensen Emiel, Liu Peng. Unveiling the Au-Mn-Cu synergy in Au/LaMnCuO₃ catalysts for selective ethanol oxidation[J]. Chinese Journal of Catalysis, 2025, 75: 34-48.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64686-9

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Figures/Tables 14

Table 1 Textural, structural and chemical properties of perovskite-supported Au catalysts.

Catalyst	S_BET (m² g^-1)	d_Au ^a (nm)	[Au] ^b (wt%)	XPS peak area ratio (%)			H₂ uptake ^c (mmol g^-1)	Acid amount ^d (μmol g^-1)	Base amount ^e (μmol g^-1)
Catalyst	S_BET (m² g^-1)	d_Au ^a (nm)	[Au] ^b (wt%)	(O_A+O_V)/O_L	Mn³⁺/Mn	Cu⁺/Cu	H₂ uptake ^c (mmol g^-1)	Acid amount ^d (μmol g^-1)	Base amount ^e (μmol g^-1)
Au/LaMnO₃	5.3	3.0	0.96	48.4	69.6	—	3.3 (3.3)	80.7	150.8
Au/LaMn_0.75Cu_0.25O₃	2.2	3.5	0.95	60.3	63.6	10.0	3.6 (3.5)	15.3	50.7
Au/LaMn_0.5Cu_0.5O₃	1.0	4.0	0.99	80.0	58.1	9.3	3.8 (3.9)	13.6	39.1
Au/La₂CuO₄	0.5	6.5	0.98	481.3	—	0	4.5 (4.6)	12.1	31.5

Fig. 1. SEM images (A), TEM images (B), AuNP size distributions (C), and XRD patterns (D) of (a) Au/LaMnO3, (b) Au/LaMn0.75Cu0.25O3, (c) Au/LaMn0.5Cu0.5O3, and (d) Au/La2CuO4.

Fig. 2. XPS spectra of the Au/LaMnO3 (a), Au/LaMn0.75Cu0.25O3 (b) and Au/La2CuO4 (c) catalysts. (A) La 3d; (B) Au 4f, Mn 3s; (C) O 1s; (D) Mn 2p; (E) Cu 2p; (F) Auger Cu LMM.

Fig. 3. H2-TPR profiles of various perovskite-supported Au catalysts and the corresponding perovskite supports (the dashed line).

Table 2 Catalytic performance of supported Au catalysts in the aerobic ethanol oxidation.

Catalyst	Conv. ^a (%)	Selec. ^a (%)	STY ^b (h^-1)	TOF ^c (h^-1)	E_a ^d (kJ mol^-1)
Au/LaMnO₃	99	1	4	162	76.1
Au/LaMn_0.75Cu_0.25O₃	97	98	378	1580	40.1
Au/LaMn_0.5Cu_0.5O₃	67	97	248	368	47.7
Au/La₂CuO₄	50	99	191	517	51.9
Au/MgCuCr₂O₄	82	99	329	1039	45.0
Au/La₂O₃	28	81	93	205	83.2
Au/β-MnO₂	99	1	4	421	56.5
Au/CuO	48	96	181	406	78.7

Fig. 4. Ethanol conversion (A), AC selectivity (B) and yield (C) as a function of the reaction temperature, and (D) Arrhenius plots for ethanol oxidation, and (E) a stability test for Au/LaMn0.75Cu0.25O3. Reaction conditions: catalyst 0.06 g, ethanol 5.0 μL min-1, ethanol/O2/N2 = 1/3/36, GHSV = 100000 mL gcat-1 h-1).

Fig. 5. XPS spectra of fresh (a) and used (b) Au/LaMn0.75Cu0.25O3 catalysts. (A) La 3d; (B) Au 4f and Mn 3s; (C) O 1s; (D) Mn 2p; (E) Cu 2p; (F) Auger Cu LMM.

Fig. 6. Effect of Au loading of the Au/LaMn0.75Cu0.25O3 catalyst (I: 0.95 wt% Au, II: 0.47 wt% Au, III: 0.17 wt% Au) on the activity and selectivity (A) and STY value (B) for the ethanol oxidation. Reaction conditions: catalyst 0.06 g, ethanol 5.0 μL min-1, ethanol/O2/N2 = 1/3/36, GHSV = 100000 mL gcat-1 h-1).

Fig. 7. Surface models of optimized Au8 clusters on the (001) surfaces of LaMnO3 (A), LaMnCuO3 (B) and La2MnO4 (C). color coding: blue for La, purple for Mn, red for O, gold for Au, and olive for Cu.

Fig. 8. The Mars-van Krevelen mechanism of selective oxidation of ethanol (color codes: dark gray round rectangular: supports; gold: Au; black: C; red: O in ethanol; white: H; pink circle with black border: lattice O; pink circle with white border: absorbed O). The activation energy of each elementary step is indicated, with black, red and green representing values for Au/LaMnO3, Au/LaMnCuO3, and Au/La2CuO4, respectively. Values to the left and right of the vertical bars denote the activation energies in eV of the forward and backward reactions, respectively.

Table 3 DFT-computed activation energies of elementary reaction steps in selective ethanol oxidation on the Au/LaMnO3, Au/LaMnCuO3 and Au/La2CuO4 surface models (all energies in eV and corrected for the zero-point energy).

Reaction step		Au/LaMnO₃		Au/LaMnCuO₃		Au/La₂CuO₄
Reaction step		Forward	Backward	Forward	Backward	Forward	Backward
R1	CH₃CH₂OH + * ⇋ CH₃CH₂OH*	0	0.79	0	0.94	0	0.72
R2	CH₃CH₂OH* ⇋ CH₃CH₂OOHO_v*	0.06	0.04	0.28	0.30	0.33	0.24
R3	CH₃CH₂OOHO_v ⇋ CH₃CHOHOHO_v	0.67	0.50	0.39	0.32	0.91	0.82
R4	CH₃CHO* + HOHO_v* ⇋ CH₃CHOHOHO_v	0	0.93	0	0.97	0	0.27
R5	HOHO_v ⇋ H₂OO_v	0.97	1.06	0.70	0.60	0.79	0.91
R6	H₂O + O_v* ⇋ H₂OO_v	0	0.86	0	0.17	0	0.57
R7	O₂ + O_v* ⇋ O₂O_v	0	1.85	0	1.27	0	0.95
R8	CH₃CH₂OH + O₂O_v ⇋ CH₃CH₂OHO₂O_v	0	1.18	0	0.86	0	0.76
R9	CH₃CH₂OHO₂O_v* ⇋ CH₃CH₂OOH	0.06	2.00	0.38	1.21	0.73	0.98
R10	CH₃CH₂OOH ⇋ CH₃CHOHOH*	1.28	0.24	0.68	1.35	0.83	1.90
R11	CH₃CHO* + HOH ⇋ CH₃CHOHOH*	0	0.48	0	0.79	0	0.84
R12	HOH ⇋ H₂O*	1.67	2.81	0.72	1.59	0.57	1.91
R13	H₂O + * ⇋ H₂O*	0	0.57	0	0.54	0	0.43

Fig. 9. Microkinetics simulations of the ethanol conversion rate (conditions: ethanol/O2/N2 = 1/3/36, P = 1 atm) (A) and the degree of rate control as a function of temperature on Au/LaMnO3 (B), Au/LaMnCuO3 (C) and Au/La2CuO4 (D).

Fig. 10. Steady-state surface coverages, reaction orders and apparent activation energy as a function of temperature for Au/LaMnO3 (A,D), Au/LaMnCuO3 (B,E), and Au/La2CuO4 (C,F).

Table 4 iCOHP and ?iCOHP values for the key interactions in H2O formation reaction over Au/LaMnO3 and Au/LaMnCuO3 models.

Interaction	Au/LaMnO₃			Au/LaMnCuO₃
Interaction	iCOHP_IS	iCOHP_TS	∆iCOHP	iCOHP_IS	iCOHP_TS	∆iCOHP
Mn-O/Cu-O	-1.65	-1.53	0.12	-1.47	-0.68	0.79
Au-O	-1.28	-0.36	0.92	-1.43	-0.76	0.67
Au-H	-2.49	-2.48	0.01	-3.68	-2.81	0.87
HO-H	-0.10	-1.24	-1.22	-0.09	-1.57	-1.48

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Unveiling the Au-Mn-Cu synergy in Au/LaMnCuO₃ catalysts for selective ethanol oxidation

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