Defect and interface engineering for promoting electrocatalytic N-integrated CO2 co-reduction

doi:10.1016/S1872-2067(23)64588-7

Chinese Journal of Catalysis ›› 2024, Vol. 57: 1-17.DOI: 10.1016/S1872-2067(23)64588-7

Defect and interface engineering for promoting electrocatalytic N-integrated CO₂ co-reduction

Zhichao Wang^a, Mengfan Wang^b^,^*(), Yunfei Huan^c, Tao Qian^c, Jie Xiong^a, Chengtao Yang^a^,^*(), Chenglin Yan^b^,^d^,^*()

^aState Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
^bCollege of Energy, Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006, Jiangsu, China
^cSchool of Chemistry and Chemical Engineering, Nantong University, Nantong 226019, Jiangsu, China
^dSchool of Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu, China

Received:2023-10-26 Accepted:2023-12-21 Online:2024-02-18 Published:2024-02-10
Contact: * E-mail: mfwang1204@suda.edu.cn (M. Wang), ctyang@uestc.edu.cn (C. Yang),c.yan@suda.edu.cn (C. Yan).
About author:Mengfan Wang is a postdoc fellow in the College of Energy at Soochow University in Suzhou, China. He received his PhD degree from Soochow University in 2021. His current research focuses on rational design of electrocatalytic systems toward gas‐involved electrochemical reactions.
Chengtao Yang is a full professor at the University of Electronic Science and Technology of China (UESTC). He received his Ph.D. degree in materials physics and chemistry from the UESTC in 2004. His research interests focus on ferroelectric/piezoelectric film materials and ferroelectric/piezo- electric integrated device, electronic ceramic materials and components, and energy materials.
Chenglin Yan (School of Petrochemical Engineering at Changzhou University) is a Professor and Vice President of the School of Petrochemical Engineering at Changzhou University in Changzhou, China. He received his Ph.D. from Dalian University of Technology in 2008. In 2011, he became a staff scientist and a group leader at the Institute for Integrative Nanoscience at the Leibniz Institute in Dresden (Germany). His primary research interests focus on electrochemical energy storage and conversion.
Supported by:
National Natural Science Foundation of China(U21A20332);National Natural Science Foundation of China(52103226);National Natural Science Foundation of China(52202275);National Natural Science Foundation of China(52203314);National Natural Science Foundation of China(12204253);Distinguished Young Scholars Fund of Jiangsu Province(BK20220061)

Abstract

Abstract:

Current industrial manufacturing producing chemicals and fertilizers usually requires harsh conditions with high energy consumption, and is thus a major contributor to global carbon dioxide (CO₂) emissions. With the increasing demand for sustainability, the scientific researchers are endeavoring to develop efficient carbon-neutral and nitrogen-cycle strategies that utilize sustainable energy storage and conversion technologies. In this context, electrocatalytic coupling of CO₂ and nitrogenous species (such as nitrogen, ammonia, nitrate, and nitrite) to high-value-added chemicals and fuels with rationally designed electrocatalysts is a promising strategy to restore the imbalanced carbon neutrality and nitrogen cycle. However, despite considerable breakthrough in recent years, the electrocatalytic N-integrated CO₂ co-reduction still suffers from the unsatisfactory activity and selectivity, as well as the ambiguous C-N coupling mechanisms. In this review, we summarize the recent progress on defect and interface engineering strategies to design highly efficient electrocatalysts for electrochemical C-N coupling. Especially, the structure-activity relationships between defect/interface engineering and electrochemical performance are systematically illustrated using representative experimental data and theoretical calculations. Moreover, the major challenge and future development direction of defect and interface engineering are also proposed. It is hoped that this work can provide guidance and enlightenment for the development of electrochemical C-N coupling technology.

Key words: C-N coupling reaction, Defect engineering, Interface engineering, Synthetic urea, CO₂ reduction

Zhichao Wang, Mengfan Wang, Yunfei Huan, Tao Qian, Jie Xiong, Chengtao Yang, Chenglin Yan. Defect and interface engineering for promoting electrocatalytic N-integrated CO₂ co-reduction[J]. Chinese Journal of Catalysis, 2024, 57: 1-17.

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Figures/Tables 10

Fig. 1. Schematic diagram of sustainable production of high-value-added chemicals from electrocatalytic N-integrated CO2 co-reduction.

Fig. 2. Schematic overview of defect and interface engineering strategies for electrocatalytic N-integrated CO2 co-reduction.

Fig. 3. SFG signals of intermediate species on pristine CeO2 (a) and VO-CeO2-750 (b). (c) Urea yield rates of CeO2 and oxygen vacancy-mediated CeO2 catalysts at different potentials. Reprinted with permission from Ref. [86]. Copyright 2022, American Chemical Society. (d) The urea synthesis performance of InOOH and VO-InOOH at -0.5 V vs. RHE. (e) Free-energy diagrams for urea synthesis on the (010) facets of InOOH and VO-InOOH. Reprinted with permission from Ref. [87]. Copyright 2022, American Chemical Society. (f) In-situ ART-FTIR spectra of ZnO-V under various electrochemical conditions. (g) Schematic illustration of urea formation over ZnO-V. (h) The urea synthesis Faradaic efficiency at different potentials over ZnO-V. Reprinted with permission from Ref. [88]. Copyright 2021, Elsevier. (i) Two Cu (111) surfaces with a spacing of ds were used to simulate copper with an atomic gap. (j) The calculated kinetic barriers for various C-N coupling reactions. Reprinted with permission from Ref. [89]. Copyright 2023, Royal Society of Chemistry.

Fig. 4. XANES (a) and EXAFS (b) spectra of Cu1-CeO2 at different potentials during C-N coupling process at Cu K-edge. (c) Schematic diagram of reconstitution of Cu single-atoms to nanoclusters. Reprinted with permission from Ref. [96]. Copyright 2023, John Wiley and Sons. CO2-TPD (d) and N2-TPD (e) spectra of Pd1-TiO2 and Pd1Cu1-TiO2. Reprinted with permission from Ref. [97]. Copyright 2023, John Wiley and Sons. (f) The structural model of F-doped CNT. Brown, red, pink, blue, and green spheres present C, O, H, F, and N atoms, respectively. (g) Free energy diagrams of C-N coupling reaction for CNT and F-CNT. Reprinted with permission from Ref. [99]. Copyright 2022, Elsevier.

Fig. 5. XANES (a) and spectra at Cu K-edge (b) for Cu-GS-800, Cu-GS-900, and Cu-GS-1000. (c) Faradaic efficiencies of as-prepared products for Cu-GS-800 under different potentials. Reprinted with permission from Ref. [108]. Copyright 2022, John Wiley and Sons. (d) Proposed “Four-Step” strategy for screening promising catalysts for urea synthesis. (e) Free energies of N2* intermediate via end/side-on pattern. (f) Volcano plot of adsorption energy of *NCON intermediate as a function of limiting potential of urea synthesis on different M/p-BN catalysts. Reprinted with permission from Ref. [109]. Copyright 2023, Elsevier.

Fig. 6. (a) High angle annular dark field scanning transmission electron microscopy image of B-FeNi-DASC. (b) Atomic-resolution electron energy-loss spectroscopy mapping of the Fe-Ni configuration. (c) Free energy diagram of urea production over B-FeNi-DASC electrocatalyst. Reprinted with permission from Ref. [112]. Copyright 2023, Springer Nature. (d) Urea yield rates and Faradaic efficiencies of ZnMn-N and ZnMn-N,Cl with CO pre-poisoning. (e) CO-TPD spectra of ZnMn-N and ZnMn-N,Cl. (f) Free energies of side/end-on adsorption of N2 over Zn-Mn catalysts. Reprinted with permission from Ref. [113]. Copyright 2023, John Wiley and Sons. Flowchart of screening procedures (g) and schematic depiction (h) of potential reaction pathways for urea generation. Reprinted with permission from Ref. [115]. Copyright 2023, John Wiley and Sons.

Fig. 7. DEMS spectra of CO (a) and NH2 (b) signals over Cu@Zn under different electrochemical conditions. Reprinted with permission from Ref. [123]. Copyright 2022, American Chemical Society. (c) The average charge density difference for Bi-BiVO4 heterojunction, yellow and cyan regions present electron accumulation and depletion, respectively. Free energy diagrams for N2 (d) and CO2 (e) adsorption on BiVO4 and Bi-BiVO4 and the corresponding structure models. Reprinted with permission from Ref. [124]. Copyright 2021, John Wiley and Sons. (f) Schematic electrocatalytic urea production mechanism on BiFeO3/BiVO4 heterojunction. Reprinted with permission from Ref. [125]. Copyright 2023, Royal Society of Chemistry.

Fig. 8. XANES (a) and EXAFS (b) spectra of Mo foil, MoO3, and MoOx/C at Mo K-edge. Reprinted with permission from Ref. [22]. Copyright 2023, John Wiley and Sons. High-resolution XPS spectra of (c) Ni 2p and (d) Co 2p for Co-NiOx and Co-NiOx@GDY. Reprinted with permission from Ref. [17]. Copyright 2022, Oxford University Press. TEM (e) and high-resolution TEM (HRTEM) (f) images of Bi2S3/N-RGO. (g) Linear sweep voltammetry curves of Bi2S3/N-RGO. (h) Urea yield rate and Faradaic efficiency of Bi2S3/N-RGO at different potentials. Reprinted with permission from Ref. [129]. Copyright 2023, American Chemical Society.

Fig. 9. (a) Schematic illustration of electrocatalytic CO2 and nitrite reduction for C-N coupling of urea production on AuCu SANFs. (b,c) TEM, selected area electron diffraction (SAED) and HRTEM images of AuCu SANFs. Reprinted with permission from Ref. [135]. Copyright 2022, Elsevier. (d) Schematic illustration of the electron transfer from Cu to Rh atoms on the RhCu-uls. Reprinted with permission from Ref. [136]. Copyright 2023, Royal Society of Chemistry. (e) Products distribution at different potentials in CO-saturated 1.0 mol L-1 KOH + 1.0 mol L-1 KNO2 electrolyte on Ru1Cu SAA. (f) Free energy diagrams for NO2? reduction with the assistance of *CO and (g) synthesis of formamide on Ru1Cu SAA surface. Reprinted with permission from Ref. [137]. Copyright 2023, Springer Nature. (h) Urea yield rates of Cu-C, Cu97In3-C, Cu30In70-C and In-C at different potentials. (i) Urea yield rates and corresponding carbon monoxide/formate ratios on bimetallic systems. Reprinted with permission from Ref. [138]. Copyright 2023, John Wiley and Sons.

Table 1 Summary of defect and interface engineering catalysts for electrocatalytic N-integrated CO2 co-reduction reaction.

Catalyst	Active site	Carbon source	Nitrogen source	Operating condition	Major product	Yield rate	Efficiency	Ref.
V_O-CeO₂-750	O vacancy	CO₂	NO₃⁻	-1.6 V vs. RHE	urea	943.6 mg h^-1 g^-1	N.A.	[86]
V_O-InOOH	O vacancy	CO₂	NO₃⁻	-0.5 V vs. RHE	urea	592.5 μg h^-1 mg^-1	51.0%	[87]
ZnO-V	O vacancy	CO₂	NO₂⁻	-0.79 V vs. RHE	urea	16.56 mmol h^-1	23.26%	[88]
V_N-Cu₃N-300	N vacancy	CO₂	N₂	-0.4 V vs. RHE	urea	81 μg h^-1 cm^-2	28.7%	[90]
6 Å-Cu	atomic-defects	CO₂	NO₃⁻	-0.4 V vs. RHE	urea	7541.9 μg h^-1 mg^-1	51.97 ± 0.8%	[89]
Cu-TiO₂	Cu doping	CO₂	NO₂⁻	-0.4 V vs. RHE	urea	20.8 μmol h^-1	43.1%	[54]
Cu-CeO₂	Cu doping	CO₂	NO₃⁻	-1.6 V vs. RHE	urea	52.84 mmol h^-1 g^-1	N.A.	[96]
Pd₁Cu₁-TiO₂	dual-atom/O vacancy	CO₂	N₂	-0.5 V vs. RHE	urea	166.67 mol_urea mol_Pd^-1 h^-1	22.54%	[97]
Te-Pd NCs	Te doping	CO₂	NO₂⁻	-1.1 V vs. RHE	urea	N.A.	12.2%	[98]
F-CNT	F doping	CO₂	NO₃⁻	-0.65 V vs. RHE	urea	6.36 mmol h^-1 g^-1	18.0%	[99]
BDD	B doping	CH₃OH	NH₃	120 mA cm^-2	formamide	36.9 g h^-1	41.2%	[101]
Cu SACs	signal atom	CO₂	NO₃⁻	-0.9 V vs. RHE	urea	4.3 nmol s^-1 cm^-2	28%	[108]
B-FeNi-DASC	dual atom	CO₂	NO₃⁻	-1.5 V vs. RHE	urea	20.2 mmol h^-1 g^-1	17.8%	[112]
ZnMn-N,Cl	dual atom	CO	NO₃⁻	-0.3 V vs. RHE	urea	4.0 mmol g^-1 h^-1	63.5%	[113]
Cu@Zn	Cu/Zn interface	CO₂	NO₃⁻	-1.02 V vs. RHE	urea	7.29 μmol cm^-2 h^-1	9.28%	[123]
Bi-BiVO₄	heterojunction	CO₂	N₂	-0.4 V vs. RHE	urea	5.91 mmol h^-1 g^-1	12.55%	[124]
BiFeO₃/BiVO₄	heterojunction	CO₂	N₂	-0.4 V vs. RHE	urea	4.94 mmol h^-1 g^-1	17.18%	[125]
CoPc-MoS₂	dual sites	CO₂	N₂	-0.7 V vs. RHE	urea	175.6 μg h^-1 mg^-1	15.12%	[126]
MoO_x/C	Mo-C interfaces	CO₂	NO₃⁻	-0.6 V vs. RHE	urea	1431.5 μg h^-1 mg^-1	27.7%	[22]
Co-NiO_x@GDY	heterojunction	CO₂	NO₂⁻	-0.7 V vs. RHE	urea	913.2 μg h^-1 mg^-1	64.3%	[17]
Bi₂O₃/N-RGO	heterojunction	CO₂	N₂	-0.5 V vs. RHE	urea	4.4 mmol g^-1 h^-1	7.5%	[129]
Fe(a)@C-Fe₃O₄/CNTs	dual sites	CO₂	NO₃⁻	-0.65 V vs. RHE	urea	1341.3 ± 112.6 μg h^-1 mg^-1	16.5 ± 6.1%	[130]
Pd₁Cu₁-TiO₂	alloying	CO₂	N₂	-0.4 V vs. RHE	urea	3.36 mmol g^-1 h^-1	8.92%	[134]
AuCu SANFs	alloying	CO₂	NO₂⁻	-1.55 V vs. Ag/AgCl	urea	3889.6 μg h^-1 mg^-1	24.7%	[135]
RhCu	alloying	CO₂	NO₃⁻	-0.6 V vs. RHE	urea	26.81 ± 0.62 mmol g^-1 h^-1	34.82 ± 2.47%	[136]
Ru₁Cu SAA	alloying	CO	NO₂⁻	-0.5 V vs. RHE	formamide	2483.77 ± 155.34 μg h^-1 mg^-1	45.65 ± 0.76%	[137]
Cu₉₇In₃-C	alloying	CO₂	NO₃⁻	-1.4 V vs. RHE	urea	13.1 mmol g^-1 h^-1	N.A.	[138]
Cu-Hg alloys	alloying	oxalic acid	NO₃⁻	-1.4 V vs. Ag/AgCl	glycine	N.A.	43.1%	[139]

Table 1 Summary of defect and interface engineering catalysts for electrocatalytic N-integrated CO2 co-reduction reaction.

Catalyst	Active site	Carbon source	Nitrogen source	Operating condition	Major product	Yield rate	Efficiency	Ref.
V_O-CeO₂-750	O vacancy	CO₂	NO₃⁻	-1.6 V vs. RHE	urea	943.6 mg h^-1 g^-1	N.A.	[86]
V_O-InOOH	O vacancy	CO₂	NO₃⁻	-0.5 V vs. RHE	urea	592.5 μg h^-1 mg^-1	51.0%	[87]
ZnO-V	O vacancy	CO₂	NO₂⁻	-0.79 V vs. RHE	urea	16.56 mmol h^-1	23.26%	[88]
V_N-Cu₃N-300	N vacancy	CO₂	N₂	-0.4 V vs. RHE	urea	81 μg h^-1 cm^-2	28.7%	[90]
6 Å-Cu	atomic-defects	CO₂	NO₃⁻	-0.4 V vs. RHE	urea	7541.9 μg h^-1 mg^-1	51.97 ± 0.8%	[89]
Cu-TiO₂	Cu doping	CO₂	NO₂⁻	-0.4 V vs. RHE	urea	20.8 μmol h^-1	43.1%	[54]
Cu-CeO₂	Cu doping	CO₂	NO₃⁻	-1.6 V vs. RHE	urea	52.84 mmol h^-1 g^-1	N.A.	[96]
Pd₁Cu₁-TiO₂	dual-atom/O vacancy	CO₂	N₂	-0.5 V vs. RHE	urea	166.67 mol_urea mol_Pd^-1 h^-1	22.54%	[97]
Te-Pd NCs	Te doping	CO₂	NO₂⁻	-1.1 V vs. RHE	urea	N.A.	12.2%	[98]
F-CNT	F doping	CO₂	NO₃⁻	-0.65 V vs. RHE	urea	6.36 mmol h^-1 g^-1	18.0%	[99]
BDD	B doping	CH₃OH	NH₃	120 mA cm^-2	formamide	36.9 g h^-1	41.2%	[101]
Cu SACs	signal atom	CO₂	NO₃⁻	-0.9 V vs. RHE	urea	4.3 nmol s^-1 cm^-2	28%	[108]
B-FeNi-DASC	dual atom	CO₂	NO₃⁻	-1.5 V vs. RHE	urea	20.2 mmol h^-1 g^-1	17.8%	[112]
ZnMn-N,Cl	dual atom	CO	NO₃⁻	-0.3 V vs. RHE	urea	4.0 mmol g^-1 h^-1	63.5%	[113]
Cu@Zn	Cu/Zn interface	CO₂	NO₃⁻	-1.02 V vs. RHE	urea	7.29 μmol cm^-2 h^-1	9.28%	[123]
Bi-BiVO₄	heterojunction	CO₂	N₂	-0.4 V vs. RHE	urea	5.91 mmol h^-1 g^-1	12.55%	[124]
BiFeO₃/BiVO₄	heterojunction	CO₂	N₂	-0.4 V vs. RHE	urea	4.94 mmol h^-1 g^-1	17.18%	[125]
CoPc-MoS₂	dual sites	CO₂	N₂	-0.7 V vs. RHE	urea	175.6 μg h^-1 mg^-1	15.12%	[126]
MoO_x/C	Mo-C interfaces	CO₂	NO₃⁻	-0.6 V vs. RHE	urea	1431.5 μg h^-1 mg^-1	27.7%	[22]
Co-NiO_x@GDY	heterojunction	CO₂	NO₂⁻	-0.7 V vs. RHE	urea	913.2 μg h^-1 mg^-1	64.3%	[17]
Bi₂O₃/N-RGO	heterojunction	CO₂	N₂	-0.5 V vs. RHE	urea	4.4 mmol g^-1 h^-1	7.5%	[129]
Fe(a)@C-Fe₃O₄/CNTs	dual sites	CO₂	NO₃⁻	-0.65 V vs. RHE	urea	1341.3 ± 112.6 μg h^-1 mg^-1	16.5 ± 6.1%	[130]
Pd₁Cu₁-TiO₂	alloying	CO₂	N₂	-0.4 V vs. RHE	urea	3.36 mmol g^-1 h^-1	8.92%	[134]
AuCu SANFs	alloying	CO₂	NO₂⁻	-1.55 V vs. Ag/AgCl	urea	3889.6 μg h^-1 mg^-1	24.7%	[135]
RhCu	alloying	CO₂	NO₃⁻	-0.6 V vs. RHE	urea	26.81 ± 0.62 mmol g^-1 h^-1	34.82 ± 2.47%	[136]
Ru₁Cu SAA	alloying	CO	NO₂⁻	-0.5 V vs. RHE	formamide	2483.77 ± 155.34 μg h^-1 mg^-1	45.65 ± 0.76%	[137]
Cu₉₇In₃-C	alloying	CO₂	NO₃⁻	-1.4 V vs. RHE	urea	13.1 mmol g^-1 h^-1	N.A.	[138]
Cu-Hg alloys	alloying	oxalic acid	NO₃⁻	-1.4 V vs. Ag/AgCl	glycine	N.A.	43.1%	[139]

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Defect and interface engineering for promoting electrocatalytic N-integrated CO₂ co-reduction

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