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学者姓名：颜蔚
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Abstract ：
Electrocatalytic C-N coupling reaction is regarded as a promising strategy for achieving clean and sustainable urea production by coreducing CO2 and nitrogen species, thus contributing to carbon neutrality and the artificial nitrogen cycle. However, restricted by the sluggish adsorption of reactants, competitive side reactions, and multistep reaction pathways, the electrochemical urea production suffers from a low urea yield rate and low selectivity so far. In order to comprehensively improve urea synthesis performance, it is crucial to develop highly efficient catalysts for electrochemical C-N coupling. In this article, the catalyst-designing strategies, C-N coupling mechanisms, and fundamental research methods are reviewed. For the coreduction of CO2 and different nitrogen species, several prevailing reaction mechanisms are discussed. With the aim of establishing the standard research system, the fundamentals of electrocatalytic urea synthesis research are introduced. The most important catalyst-designing strategies for boosting the electrocatalytic urea production are discussed, including heteroatom doping, vacancy engineering, crystal facet regulation, atom-scale modulation, alloying and heterostructure construction. Finally, the challenges and perspectives are proposed for future industrial applications of electrochemical urea production by C-N coupling. The rational design of efficient heterogeneous electrocatalysts is crucial but still very challenging for sustainable urea production at ambient conditions by coreducing CO2 and nitrogen species. In this review article, design strategies for C-N coupling electrocatalysts are emphasized-for the in-depth understanding of the structure-activity relationship and the establishment of a systematic research framework -toward this emerging field. image
Keyword ：
artificial nitrogen cycle artificial nitrogen cycle carbon neutrality carbon neutrality catalyst-designing strategies catalyst-designing strategies C-N coupling C-N coupling electrocatalytic urea synthesis electrocatalytic urea synthesis
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| GB/T 7714 | Wan, Yuchi , Zheng, Muyun , Yan, Wei et al. Fundamentals and Rational Design of Heterogeneous C-N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions [J]. | ADVANCED ENERGY MATERIALS , 2024 , 14 (28) . |
| MLA | Wan, Yuchi et al. "Fundamentals and Rational Design of Heterogeneous C-N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions" . | ADVANCED ENERGY MATERIALS 14 . 28 (2024) . |
| APA | Wan, Yuchi , Zheng, Muyun , Yan, Wei , Zhang, Jiujun , Lv, Ruitao . Fundamentals and Rational Design of Heterogeneous C-N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions . | ADVANCED ENERGY MATERIALS , 2024 , 14 (28) . |
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Carbon defects coupled with heteroatoms can asymmetrically rearrange the local electronic distribution and coordination environment of active sites, improving the catalytic selectivity and activity of a two-electron oxygen reduction reaction (2eORR). In this study, an asymmetry defective carbon (asy-DC) structure using wolfberry as the carbon source is employed to adjust the charge distribution of active sites with different degrees of asymmetry caused by N→S coordination bonds. The asymmetric region exhibits a considerable positive correlation between the asymmetry degree and adsorption energy for OOH*, presenting a volcano relation between the asymmetry degree and catalytic activity. The optimised asy-DC catalyst exhibits high selectivity and reliable activity after 12 h of stability testing. This study can provide a new reference into the origin of ORR activity and selectivity. © 2024 Elsevier B.V.
Keyword ：
2eORR 2eORR Asymmetry Asymmetry Carbon defect Carbon defect Catalytic activity Catalytic activity Charge redistribution Charge redistribution
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| GB/T 7714 | Zhai, Z. , Wang, Y.-J. , Pan, L. et al. Asymmetric structures to switch on the selective oxygen reduction to hydrogen peroxide [J]. | Journal of Alloys and Compounds , 2024 , 1003 . |
| MLA | Zhai, Z. et al. "Asymmetric structures to switch on the selective oxygen reduction to hydrogen peroxide" . | Journal of Alloys and Compounds 1003 (2024) . |
| APA | Zhai, Z. , Wang, Y.-J. , Pan, L. , Zhu, Z. , Yan, W. , Wang, B. et al. Asymmetric structures to switch on the selective oxygen reduction to hydrogen peroxide . | Journal of Alloys and Compounds , 2024 , 1003 . |
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CO and H 2 S poisoning of Pt -based catalysts for hydrogen oxidation reaction (HOR) stands as one of the longstanding hindrances to the widespread commercialization of proton exchange membrane fuel cells. In this paper, a Ru/Ti 4 O 7 catalyst is successfully synthesized by the microwave -thermal method. This Ru/Ti 4 O 7 catalyst shows a much higher noble metal mass activity than those of commercial PtRu/C and conventional Ru/C catalysts. The performance of the Ru/Ti 4 O 7 catalyst under the exist of CO or H 2 S shows insignificant current decay, which is far superior to commercial PtRu/C and Pt/C catalysts. In this Ru/Ti 4 O 7 catalyst, the electron transfer between Ru and Ti to form d -p orbital hybridization is considered to be responsible for the favorable catalytic HOR performance and the corresponding CO and H 2 S tolerance. The interaction mechanism formed by electron transfer may open a promising way for the subsequent development of anti -poisoning catalysts for PEM fuel cell hydrogen oxidation reaction.
Keyword ：
CO poisoning CO poisoning H2 H2 Hydrogen oxidation reaction Hydrogen oxidation reaction PEM fuel cell PEM fuel cell
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| GB/T 7714 | Xie, Yujie , Lian, Bianyong , Deng, Shuqi et al. Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2024 , 65 : 205-214 . |
| MLA | Xie, Yujie et al. "Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 65 (2024) : 205-214 . |
| APA | Xie, Yujie , Lian, Bianyong , Deng, Shuqi , Lin, Qingqu , Wang, Kaili , Zheng, Yun et al. Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2024 , 65 , 205-214 . |
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The large overpotential required for oxygen evolution reaction (OER) is one of the major factors limiting the efficiency of electrochemical water-electrolysis for hydrogen production. In this work, to decrease OER energy barrier and obtain low overpotential, amorphous-crystalline NiCo(OH)2 nanoplates are in-situ grown on nickel foam surface to form a catalyst-based electrode (ac-NiCo(OH)2/NF) for water-electrolysis application. As the inner amorphization of NiCo(OH)2 results in increased electron density of the metal sites, leading to the formation of tensile Ni-O bond, the coordinatively unsaturated Ni sites in the down-shift d-band centers toward Fermi level can lower the anti-bonding states. This can lead to optimized adsorption and desorption energies for oxygen-containing intermediates for OER. As expected, the prepared ac-NiCo(OH)2/NF electrode presents a low overpotential of 364 mV to deliver 1000 mA cm-2 toward OER with impressively high robust stability. When this electrocatalyst electrode serves as both the anode and cathode, the assembled anion exchange membrane (AEM) electrolyser only needs a cell voltage of 1.68 V to drive the overall water-electrolysis process at a current density of 10 mA cm-2.
Keyword ：
AEM electrolyser AEM electrolyser Amorphous-crystalline Amorphous-crystalline High current density High current density Oxygen evolution Oxygen evolution Unsaturated atoms Unsaturated atoms
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| GB/T 7714 | Ju, Shang , Liu, Yao , Pei, Maojun et al. Amorphization-induced abundant coordinatively unsaturated Ni active sites in NiCo(OH)2 for boosting catalytic OER and HER activities at high current densities for water-electrolysis [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 653 : 1704-1714 . |
| MLA | Ju, Shang et al. "Amorphization-induced abundant coordinatively unsaturated Ni active sites in NiCo(OH)2 for boosting catalytic OER and HER activities at high current densities for water-electrolysis" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 653 (2024) : 1704-1714 . |
| APA | Ju, Shang , Liu, Yao , Pei, Maojun , Shuai, Yankang , Zhai, Zibo , Yan, Wei et al. Amorphization-induced abundant coordinatively unsaturated Ni active sites in NiCo(OH)2 for boosting catalytic OER and HER activities at high current densities for water-electrolysis . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 653 , 1704-1714 . |
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Developing advanced anode materials for sodium-ion batteries (SIBs) is a frontier and hotspot research for clean and sustainable electricity energy storage and conversion. However, it is still challenging to obtain anode materials with high stability, multiple active sites, and high conductivity. In this paper, an advanced metal–organic framework (MOF)-based anode material (Co-HITP), which integrates multiple advantages into one, is successfully synthesized through a sodiation-stimulated in situ reconstruction. The Co-HITP possesses a stable single-crystal structure, expanded spacing layers, abundant sites, and good conductivity, and exhibits superior properties with ultra-long cycling stability (ultralow decay rate ≈0.001% per cycle after 15 000 cycles at 8 A g−1), high reversible capacity (450.1 mA h g−1 at 0.2 A g−1), and excellent rate performance. Both experimental results and theoretical calculation reveal that the anode remains a stable structure after long cycling, attributed to the single-crystal structure with d-π hybridization and π–π interaction, and the minimum structural unit stores 6Na+ ions of C═N sites and 8Na+ ions of aromatic rings. This discovery is significant for developing advanced anode materials with integrated advantages for SIBs. © 2024 Wiley-VCH GmbH.
Keyword ：
anode anode conductive metal–organic framework conductive metal–organic framework sodium-ion battery sodium-ion battery ultra-long cycling stability ultra-long cycling stability
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| GB/T 7714 | Shuang, W. , Wang, Y. , Wu, Y. et al. An Advanced Anode Composed of Layered Single-Crystal Metal–Organic Framework Material for Ultra-Long Cycle-Life Sodium-Ion Batteries [J]. | Advanced Functional Materials , 2024 , 34 (49) . |
| MLA | Shuang, W. et al. "An Advanced Anode Composed of Layered Single-Crystal Metal–Organic Framework Material for Ultra-Long Cycle-Life Sodium-Ion Batteries" . | Advanced Functional Materials 34 . 49 (2024) . |
| APA | Shuang, W. , Wang, Y. , Wu, Y. , Ma, N. , Chen, F. , Wang, X. et al. An Advanced Anode Composed of Layered Single-Crystal Metal–Organic Framework Material for Ultra-Long Cycle-Life Sodium-Ion Batteries . | Advanced Functional Materials , 2024 , 34 (49) . |
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Urea oxidation reaction (UOR) emerges as a promising alternative anodic half-reaction to oxygen evolution reaction (OER) in an electrochemical CO2 reduction reaction (ECRR) system. Herein, a Ni/MnO heterojunction with extraordinary UOR activity is synthesized on Ni foam. Ex situ/in situ characterization and theoretical calculation reveal that the outstanding UOR performance of Ni/MnO catalyst can be ascribed to two successive surface reconstructions. In the first and second surface reconstructions, Ni(OH)2/MnOOH and NiOOH/MnOOH heterojunctions are formed on the catalyst surface, and Mn and Ni sites serve as the active sites, respectively. The heterojunctions formed can enhance UOR activity by reducing the surface reconstruction potential and optimizing the adsorption energy of intermediates through electronic structure modulation and d-band center regulation. When employed as the UOR anode in the CO2 electrolyzer, it requires 375 mV less voltage at 10 mA cm-2 than the OER, revealing the great potential of applying such Ni/MnO catalyst as the anodic UOR in an ECRR system for carbon neutrality. © 2024 American Chemical Society.
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| GB/T 7714 | Wang, K. , Pei, M. , Shuai, Y. et al. Rapid Two Surface Reconstructions of Ni/MnO Heterojunction for Superior Urea Electrolysis [J]. | ACS Energy Letters , 2024 , 9 (9) : 4682-4690 . |
| MLA | Wang, K. et al. "Rapid Two Surface Reconstructions of Ni/MnO Heterojunction for Superior Urea Electrolysis" . | ACS Energy Letters 9 . 9 (2024) : 4682-4690 . |
| APA | Wang, K. , Pei, M. , Shuai, Y. , Liu, Y. , Deng, S. , Zhuang, Z. et al. Rapid Two Surface Reconstructions of Ni/MnO Heterojunction for Superior Urea Electrolysis . | ACS Energy Letters , 2024 , 9 (9) , 4682-4690 . |
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The uncontrollable growth of lithium dendrites and the flammability of electrolytes are the direct impediments to the commercial application of high-energy-density lithium metal batteries (LMBs). Herein, this study presents a novel approach that combines microencapsulation and electrospinning technologies to develop a multifunctional composite separator (P@AS) for improving the electrochemical performance and safety performance of LMBs. The P@AS separator forms a dense charcoal layer through the condensed-phase flame retardant mechanism causing the internal separator to suffocate from lack of oxygen. Furthermore, it incorporates a triple strategy promoting the uniform flow of lithium ions, facilitating the formation of a highly ion-conducting solid electrolyte interface (SEI), and encouraging flattened lithium deposition with active SiO2 seed points, considerably suppressing lithium dendrites growth. The high Coulombic efficiency of 95.27% is achieved in Li–Cu cells with additive-free carbonate electrolyte. Additionally, stable cycling performance is also maintained with a capacity retention rate of 93.56% after 300 cycles in LFP//Li cells. Importantly, utilizing P@AS separator delays the ignition of pouch batteries under continuous external heating by 138 s, causing a remarkable reduction in peak heat release rate and total heat release by 23.85% and 27.61%, respectively, substantially improving the fire safety of LMBs. © 2024 Wiley-VCH GmbH.
Keyword ：
dendrite-free dendrite-free fire safety fire safety flame retardant flame retardant lithium metal batteries lithium metal batteries multifunctional separator multifunctional separator
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| GB/T 7714 | Liao, C. , Li, W. , Han, L. et al. Microcapsule Modification Strategy Empowering Separator Multifunctionality to Enhance Safety of Lithium-Metal Batteries [J]. | Small , 2024 , 20 (43) . |
| MLA | Liao, C. et al. "Microcapsule Modification Strategy Empowering Separator Multifunctionality to Enhance Safety of Lithium-Metal Batteries" . | Small 20 . 43 (2024) . |
| APA | Liao, C. , Li, W. , Han, L. , Chu, F. , Zou, B. , Qiu, S. et al. Microcapsule Modification Strategy Empowering Separator Multifunctionality to Enhance Safety of Lithium-Metal Batteries . | Small , 2024 , 20 (43) . |
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Hard carbon anodes (HCAs) possessing exceptional sodium storage properties undoubtedly represents one of the optimal choices for practicable sodium-ion batteries (SIBs). In further improving and optimizing the performance of SIBs, a systematic investigation of HCA structures in particular the microstructures of solid electrolyte interface (SEI) formed on the HCA surface and the sodium storage models is definitely needed. In this paper, the recent research progress in SIBs hard carbon anodes, the formed SEIs, the degradation mechanisms and the mitigation strategies for reducing degradation is comprehensively reviewed from three primary aspects: (1) the fundamental understanding of the sodium storage mechanisms of hard carbon in terms of the distinct modes including sodium adsorption/insertion, and pore filling within hard carbon materials; (2) based on the design, synthesis, theoretical characterization and performance optimization of new materials, the understanding of the structure-performance relationship of hard carbon anodes provides a potential approach for the design of high-performance SIBs anodes; and (3) the challenges related to the degradation of hard carbon anode and the formed SEI between its surface, and the mitigation strategies for reducing the degradation. It is anticipated that this review could provide valuable guidance for future research endeavors and commercial development related to hard carbon anodes for SIBs. © 2024 Elsevier Ltd
Keyword ：
Anodes Anodes Carbon Carbon Degradation Degradation Metal ions Metal ions Microstructure Microstructure Sodium-ion batteries Sodium-ion batteries Solid electrolytes Solid electrolytes Storage (materials) Storage (materials) Structural design Structural design
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| GB/T 7714 | Qiu, Ruoxue , Ma, Dakai , Zheng, Hui et al. Performance degradation mechanisms and mitigation strategies of hard carbon anode and solid electrolyte interface for sodium-ion battery [J]. | Nano Energy , 2024 , 128 . |
| MLA | Qiu, Ruoxue et al. "Performance degradation mechanisms and mitigation strategies of hard carbon anode and solid electrolyte interface for sodium-ion battery" . | Nano Energy 128 (2024) . |
| APA | Qiu, Ruoxue , Ma, Dakai , Zheng, Hui , Liu, Mingquan , Cai, Junming , Yan, Wei et al. Performance degradation mechanisms and mitigation strategies of hard carbon anode and solid electrolyte interface for sodium-ion battery . | Nano Energy , 2024 , 128 . |
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Keyword ：
chemical confinement chemical confinement dendrite-free dendrite-free Li-metal anode Li-metal anode lithiophilicity lithiophilicity LiZn/Li2O configuration LiZn/Li2O configuration
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| GB/T 7714 | Huaming Qian , Xiangyang Li , Qinchuan Chen et al. LiZn/Li2O Induced Chemical Confinement Enabling Dendrite‐Free Li‐Metal Anode (Adv. Funct. Mater. 19/2024) [J]. | Advanced Functional Materials , 2024 , 34 (19) : n/a-n/a . |
| MLA | Huaming Qian et al. "LiZn/Li2O Induced Chemical Confinement Enabling Dendrite‐Free Li‐Metal Anode (Adv. Funct. Mater. 19/2024)" . | Advanced Functional Materials 34 . 19 (2024) : n/a-n/a . |
| APA | Huaming Qian , Xiangyang Li , Qinchuan Chen , Wen Liu , Zhu Zhao , Zhengdong Ma et al. LiZn/Li2O Induced Chemical Confinement Enabling Dendrite‐Free Li‐Metal Anode (Adv. Funct. Mater. 19/2024) . | Advanced Functional Materials , 2024 , 34 (19) , n/a-n/a . |
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Polyimide (PI) has been recognized as a potential organic cathode for Li-ion batteries (LIBs) due to its programmable structural design, high theoretical capacity, and resource availability. However, the poor intrinsic electrical conductivity of PI means that PI-based cathodes of LIBs have inefficient energy storage performance, especially at high current densities. In this work, the molecular structure of PI is optimized to obtain a layer-stacked crystalline PI with significantly enhanced dipoles, denoted NT-B for the first time. The dipoles in this PI are induced by the electronegative carbonyl groups from the monomer biuret and further enhanced via a π-π layer stacking effect. This work is the first to verify that the co-directional dipole enhancement effect of biuret is surprisingly different from that of monomer urea. A series of ex-situ/in-situ and theoretical DFT simulations are carried out to understand the functional mechanism of such effects. The multiple enhancement effects of the dipoles synergistically promoting the generation of a strong built-in electric field (BIEF) within NT-B are proposed based on the results obtained. It is confirmed that this BIEF plays a significant role in accelerating electron transport, which enhances the electrochemical activity of LIB cathodes. This work provides a new idea for the structural design of high-performance PI cathodes for LIBs. © 2024 Elsevier B.V.
Keyword ：
BIEF BIEF Dipoles Dipoles LIBs LIBs Organic cathode Organic cathode Polyimide Polyimide
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| GB/T 7714 | Chen, W. , Chen, Y. , Li, H. et al. Multiple enhancement effects of dipoles within polyimide cathode promoting highly efficient energy storage of lithium-ion batteries [J]. | Energy Storage Materials , 2024 , 73 . |
| MLA | Chen, W. et al. "Multiple enhancement effects of dipoles within polyimide cathode promoting highly efficient energy storage of lithium-ion batteries" . | Energy Storage Materials 73 (2024) . |
| APA | Chen, W. , Chen, Y. , Li, H. , Zhang, S. , Li, D. , Yu, F. et al. Multiple enhancement effects of dipoles within polyimide cathode promoting highly efficient energy storage of lithium-ion batteries . | Energy Storage Materials , 2024 , 73 . |
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