Novel Perovskite Oxide Hybrid Nanofibers Embedded with Nanocatalysts for Highly Efficient and Durable Electrodes in Direct CO2 Electrolysis

doi:10.1007/s40820-023-01298-w

Abstract

Abstract:

The unique characteristics of nanofibers in rational electrode design enable effective utilization and maximizing material properties for achieving highly efficient and sustainable CO₂ reduction reactions (CO₂RRs) in solid oxide electrolysis cells (SOECs). However, practical application of nanofiber-based electrodes faces challenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte. To tackle this challenge, a novel hybrid nanofiber electrode, La_0.6Sr_0.4Co_0.15Fe_0.8Pd_0.05O₃₋_δ (H-LSCFP), is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique. After consecutive treatment in 100% H₂ and CO₂ at 700 °C, LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface, enhancing CO₂ adsorption. The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm⁻² in CO₂ at 800 °C and 1.5 V, setting a new benchmark among reported nanofiber-based electrodes. Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO₂RR. The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure, paving the way for further advancements and nanofiber applications in CO₂-SOECs.

Key words: Nanofbers, Fuel electrodes, Digital twinning, CO₂ reduction reaction, Solid oxide electrolysis cells

Akromjon Akhmadjonov, Kyung Taek Bae, Kang Taek Lee. Novel Perovskite Oxide Hybrid Nanofibers Embedded with Nanocatalysts for Highly Efficient and Durable Electrodes in Direct CO₂ Electrolysis[J]. Nano-Micro Letters, 2024, 16(1): 93-.

Akromjon Akhmadjonov, Kyung Taek Bae, Kang Taek Lee. [J]. Nano-Micro Letters, 2024, 16(1): 93-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-023-01298-w

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/93

Figures/Tables 8

Fig. 1 a Schematic illustration depicting the synthesizing process of LSCFP nanofibers. b SEM image of the as-electrospun LSCFP nanofibers before calcination. c TEM-EDX elemental mappings of La (cyan), Sr (green), Co (purple), Fe (dark orange), Pd (red), and O (yellow) for the calcined LSCFP nanofibers. Rietveld XRD refinement of the LSCFP nanofibers d calcined in air at 1000 °C for 2 h and e LSCFP nanofibers treated in 100% H₂ of 100 sccm at 700 °C for 2 h. (Colour figure online)

Fig. 2 a Rietveld XRD refinement of the LSCFP nanofibers consecutively heat treated in 100% H₂ (100 sccm) and CO₂ (100 sccm) at 700 °C for 2 h each. SEM comparison images of the b pristine and c nanofibers consequently treated in 100% H₂ and CO₂ at 700 °C. d-h TEM-EDX elemental mappings of La (cyan), Sr (green), Co (purple), Fe (dark orange), and Pd (red). i Magnified STEM image of exsolved Co nanoparticle with HR-TEM image of j the particle and k LSCFP perovskite matrix. (Colour figure online)

Table 1 Lattice parameters derived from Rietveld refinement of LSCFP nanofibers at different states

Material	State	Phase	Crystal system	Space group	a [Å]	b [Å]	c [Å]	a [Å³]	R_wp	R_p	Χ²
LSCFP	Pristine	La_0.6Sr_0.4Co_0.2Fe_0.8O₃₋_δ	Trigonal	R-3c (167)	5.50	5.50	13.39	351.86	12.95	8.79	0.94
	Reduced	LaSrFeO₄	Tetragonal	I4/mmm (139)	3.88	3.88	12.72	192.44
		Co-Fe	Cubic	Pm-3m (221)	2.86	2.86	2.86	23.54	12.35	8.96	0.95
		Pd	Cubic	Fm-3m (225)	3.95	3.95	3.95	61.94
	Reduced & CO₂ treated	(La_0.6Sr_0.4)FeO_2.71	Trigonal	R-3c (167)	5.54	5.54	13.58	362.15
		Co	Cubic	Fm-3m (225)	3.69	3.69	3.69	50.2	5.3	4.03	1.72
		Pd	Cubic	Fm-3m (225)	3.9	3.9	3.9	59.28

Fig. 3 The oxidation state analysis of the LSCFP nanofibers calcined in air (1000 °C for 2 h) and LSCFP nanofibers after consecutive treatment in 100% H₂ and CO₂ (700 °C for 2 h each). High-resolution XPS scans of a Co 2p, b Pd 3d, and c O 1s and d corresponding CO₂-TPD profiles

Fig. 4 SEM images of the LSGM-supported symmetric cells with a H-LSCFP electrode with hybrid and F-LSCFP electrode with 100% nanofiber structures. b Temperature dependence of the interfacial polarization resistance (R_p) of both electrodes determined from the impedance data measured between 700 and 850 °C. c The impedance spectra of the electrodes in 100% CO₂ (50 sccm) at 700 °C, 1.5 V and d the corresponding DRT functions. e Stability test of the LSGM-supported symmetrical cell with H-LSCFP electrode at 800 °C in 100% CO₂

Fig. 5 a I-V curves of the LSGM-supported singles cells with H-LSCFP and F-LSCFP electrodes at 800 °C under 100% CO₂ of 50 sccm and b the corresponding Nyquist plots (inset: Bode plots). c Potentiostatic tests of the corresponding cells. d Electrochemical performance comparison in current density obtained at 1.5 V with the reported high-performance fuel electrodes. e Faradaic efficiency and CO production rate during the CO₂RR of the SOEC with the H-LSCFP fuel electrode within an applied potential range of 1.2-1.5 V, in 100% CO₂ of 50 sccm. f Stability test of the LSGM-supported single cell with the H-LSCFP electrode in 100% CO₂ at 800 °C and 1.3 V and g magnified microstructure SEM image of the corresponding cell. h Raman spectra collected from H-LSCFP electrode after 100 h long-term analysis

Table 2 A comparison of current density values obtained during CO₂ electrolysis at 800 °C and 1.5 V between various perovskite-based and Ni-based fuel electrodes

Cell configuration				Maximum current density at 1.5 V (A cm²)				Refs.
Air electrode	Electrolyte	Buffer layer	Fuel electrode	850 °C	800 °C	750 °C	700 °C	Refs.
LSCF-GDC	LSGM^b	LDC^e	H-LSCFP^c	3.7	2.2	1.37	0.76	This work
SSC^l	LSGM^b	LDC^e	LSCM^f-CMF^h	2.56	1.6	1.0	-	[1]
LSCF^a	LSGM^d	LDC	Cu@LSTMC^k	2.0	1.65	1.2	-	[47]
LSCF^a-SDCⁱ	LSGM^d	-	SFMM0.1^r-SDCⁱ	1.78	1.3	0.91	0.46	[48]
LSCF^a-GDC^j	LSGM^b	LDC^g	Fe@PSFM^m	0.85	0.7	0.58	0.45	[4]
LSCF^a-SDCⁱ	LSGM^b	LDC^e	SF1.5M^o-R	-	1.5	0.9	0.5	[3]
LSCF-SDC	LSGM	LDC	F-SFMⁿ	-	1.36	0.93	0.62	[6]
BLC^s	LSGM^d	-	Ni-Fe-LSFM^p	-	1.5	-	0.6	[16]
LSCF^a-GDC	YSZ	-	LSFNF0.1^q-GDC	1.25	0.9	0.6	-	[34]

Fig. 6 a 3D reconstructed architecture and magnified 3D microstructure image of the H-LSCFP electrode composed of LSCFP nanofibers and LSCFP crushed fibers. b Detailed view comparing TPB between the H-LSCFP and F-LSCFP at the electrode/buffer layer interface. c Quantitative comparison of the microstructural and electrochemical properties of the H-LSCFP and H-LSCSFP electrodes using a radar plot

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