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学者姓名：孙凯安
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Abstract ：
Layered double hydroxide (LDH) materials have been of interest as the noble metal substitutes for oxygen evolution reaction (OER) in alkaline media though their intrinsically inferior electrocatalytic activity. Proper cation vacancy engineering of LDH is an effective approach for improving intrinsic activity during catalytic OER. In this work, the in-situ formation of cation vacancies in LDH nanosheets (NiFeCoZnvac-LDH) is successfully realized by partially Zn etching from medium-entropy NiFeCoZn-LDH precursor. In-situ Raman analysis and DFT calculations uncover that the introduction of metal cation vacancies can significantly lower the generation potential of the surface reconstruction for the formation of abundant high-valence active centers and optimize the adsorption/desorption energy of oxygen-containing intermediates, thereby boosting catalytic OER activity. As a proof of concept, the obtained NiFeCoZnvac-LDH catalyst just requires a low overpotential of 222 mV to reach a current density of 10 mA cm-2 with a small Tafel slope of 37.17 mV dec-1. Furthermore, the NiFeCoZnvac-LDH electrode takes an ultralow potential of 1.48 V at 10 mA cm- 2 in practical anion exchange membrane electrolyzer and operate stably at 100 mA cm- 2 for long period without obvious activity attenuation. The present study enables the development of LDH catalysts for efficient water oxidation using a simple and robust approach.
Keyword ：
Active center Active center Cation vacancy Cation vacancy Layered double hydroxide Layered double hydroxide Oxygen evolution reaction Oxygen evolution reaction Surface reconstruction Surface reconstruction
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| GB/T 7714 | Wang, Kaili , Shuai, Yankang , Deng, Shuqi et al. Cation vacancy engineering in medium-entropy NiFeCoZn layered double hydroxides electrocatalysts for boosting oxygen evolution reaction in water-splitting [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 508 . |
| MLA | Wang, Kaili et al. "Cation vacancy engineering in medium-entropy NiFeCoZn layered double hydroxides electrocatalysts for boosting oxygen evolution reaction in water-splitting" . | CHEMICAL ENGINEERING JOURNAL 508 (2025) . |
| APA | Wang, Kaili , Shuai, Yankang , Deng, Shuqi , Lian, Bianyong , Zhao, Zihan , Chen, Jinghong et al. Cation vacancy engineering in medium-entropy NiFeCoZn layered double hydroxides electrocatalysts for boosting oxygen evolution reaction in water-splitting . | CHEMICAL ENGINEERING JOURNAL , 2025 , 508 . |
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Abstract ：
Developing asymmetric heteronuclear dual-atom catalysts (DACs) through coordination microenvironment regulation and investigating their structure-activity relationship for the catalytic oxygen reduction reaction (ORR) are crucial for energy conversion and storage devices such as zinc-air batteries (ZABs). In this work, a novel catalyst with its Fe and Zn diatomic sites atomically dispersed on nitrogen-doped hierarchical porous carbon (FeZn-NC-800) was designed and synthesized under a cyanamide-assisted sintering atmosphere to stabilize Zn single atoms in the structure. Benefiting from specific synergy between the Fe and Zn atoms and the hierarchical porous carbon substrate, the obtained FeZn-NC-800 catalyst exhibits remarkable ORR performance with a positive half-wave potential of 0.89 V and good durability, outstripping the performance of most state-of-the-art catalysts and commercial precious metal catalysts. Moreover, the ZABs assembled with the FeZn-NC-800 cathodes exhibit an excellent peak power density of 218.6 mW cm-2 and achieve stable cycling for over 200 hours at a current density of 10 mA cm-2. This study provides a fresh new insight into the development of stable and highly active DAC materials, advancing the design of next-generation energy technologies.
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| GB/T 7714 | Zhao, Zi-Han , Ma, Dakai , Zhuang, Zewen et al. Atomically dispersed iron-zinc dual-metal sites to boost catalytic oxygen reduction activities for efficient zinc-air batteries [J]. | NANOSCALE , 2025 , 17 (15) : 9515-9524 . |
| MLA | Zhao, Zi-Han et al. "Atomically dispersed iron-zinc dual-metal sites to boost catalytic oxygen reduction activities for efficient zinc-air batteries" . | NANOSCALE 17 . 15 (2025) : 9515-9524 . |
| APA | Zhao, Zi-Han , Ma, Dakai , Zhuang, Zewen , Wang, Kaili , Xu, Chenhui , Sun, Kaian et al. Atomically dispersed iron-zinc dual-metal sites to boost catalytic oxygen reduction activities for efficient zinc-air batteries . | NANOSCALE , 2025 , 17 (15) , 9515-9524 . |
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Abstract ：
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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Electrochemical reduction of CO2 is an important way to achieve carbon neutrality, and much effort has been devoted to the design of active sites. Apart from elevating the intrinsic activity, expanding the functionality of active sites may also boost catalytic performance. Here we designed “negatively charged Ag (nc-Ag)” active sites featuring both the intrinsic activity and the capability of regulating microenvironment, through modifying Ag nanoparticles with atomically dispersed Sn species. Different from conventional active sites (which only mediate the surface processes by bonding with the intermediates), the nc-Ag sites could also manipulate environmental species. Therefore, the sites could not only activate CO2, but also regulate interfacial H2O and CO2, as confirmed by operando spectroscopies. The catalyst delivers a high current density with a CO faradaic efficiency of 97 %. Our work here opens up new opportunities for the design of multifunctional electrocatalytic active sites. © 2024 Wiley-VCH GmbH.
Keyword ：
CO2 electro-reduction CO2 electro-reduction Microenvironment manipulation Microenvironment manipulation Multifunctional active sites Multifunctional active sites nanocatalyst nanocatalyst
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| GB/T 7714 | Dai, R. , Sun, K. , Shen, R. et al. Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions [J]. | Angewandte Chemie - International Edition , 2024 , 63 (37) . |
| MLA | Dai, R. et al. "Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions" . | Angewandte Chemie - International Edition 63 . 37 (2024) . |
| APA | Dai, R. , Sun, K. , Shen, R. , Fang, J. , Cheong, W.-C. , Zhuang, Z. et al. Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions . | Angewandte Chemie - International Edition , 2024 , 63 (37) . |
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Continuous and effective hydrogen evolution under high current densities remains a challenge for water electrolysis owing to the rapid performance degradation under continuous large-current operation. In this study, theoretical calculations, operando Raman spectroscopy, and CO stripping experiments confirm that Ru nanocrystals have a high resistance against deactivation because of the synergistic adsorption of OH intermediates (OHad) on the Ru and single atoms. Based on this conceptual model, we design the Ni single atoms modifying ultra-small Ru nanoparticle with defect carbon bridging structure (UP-RuNiSAs/C) via a unique unipolar pulse electrodeposition (UPED) strategy. As a result, the UP-RuNiSAs/C is found capable of running steadily for 100 h at 3 A cm-2, and shows a low overpotential of 9 mV at a current density of 10 mA cm-2 under alkaline conditions. Moreover, the UP-RuNiSAs/C allows an anion exchange membrane (AEM) electrolyzer to operate stably at 1.95 Vcell for 250 h at 1 A cm-2. Understanding the sustained stability of alkaline hydrogen evolution at high current densities is crucial. Herein, the authors synthesize Ni single atoms, modified with ultra-small Ru nanoparticles with a defective carbon bridging structure, capable of running steadily for 100 h at 3 A cm-2.
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| GB/T 7714 | Yao, Rui , Sun, Kaian , Zhang, Kaiyang et al. Stable hydrogen evolution reaction at high current densities via designing the Ni single atoms and Ru nanoparticles linked by carbon bridges [J]. | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
| MLA | Yao, Rui et al. "Stable hydrogen evolution reaction at high current densities via designing the Ni single atoms and Ru nanoparticles linked by carbon bridges" . | NATURE COMMUNICATIONS 15 . 1 (2024) . |
| APA | Yao, Rui , Sun, Kaian , Zhang, Kaiyang , Wu, Yun , Du, Yujie , Zhao, Qiang et al. Stable hydrogen evolution reaction at high current densities via designing the Ni single atoms and Ru nanoparticles linked by carbon bridges . | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
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Electrochemical CO2 reduction reaction (CO2RR) provides a promising route to converting CO2 into value-added chemicals and to neutralizing the greenhouse gas emission. For the industrial application of CO2RR, high-performance electrocatalysts featuring high activities and selectivities are essential. It has been demonstrated that customizing the catalyst surface/interface structures allows for high-precision control over the microenvironment for catalysis as well as the adsorption/desorption behaviors of key reaction intermediates in CO2RR, thereby elevating the activity, selectivity and stability of the electrocatalysts. In this paper, we review the progress in customizing the surface/interface structures for CO2RR electrocatalysts (including atomic-site catalysts, metal catalysts, and metal/oxide catalysts). From the perspectives of coordination engineering, atomic interface design, surface modification, and hetero-interface construction, we delineate the resulting specific alterations in surface/interface structures, and their effect on the CO2RR process. At the end of this review, we present a brief discussion and outlook on the current challenges and future directions for achieving high-efficiency CO2RR via surface/interface engineering.
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| GB/T 7714 | Tan, Xin , Zhu, Haojie , He, Chang et al. Customizing catalyst surface/interface structures for electrochemical CO2 reduction [J]. | CHEMICAL SCIENCE , 2024 , 15 (12) : 4292-4312 . |
| MLA | Tan, Xin et al. "Customizing catalyst surface/interface structures for electrochemical CO2 reduction" . | CHEMICAL SCIENCE 15 . 12 (2024) : 4292-4312 . |
| APA | Tan, Xin , Zhu, Haojie , He, Chang , Zhuang, Zewen , Sun, Kaian , Zhang, Chao et al. Customizing catalyst surface/interface structures for electrochemical CO2 reduction . | CHEMICAL SCIENCE , 2024 , 15 (12) , 4292-4312 . |
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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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Abstract ：
Electrochemical reduction of CO2 is an important way to achieve carbon neutrality, and much effort has been devoted to the design of active sites. Apart from elevating the intrinsic activity, expanding the functionality of active sites may also boost catalytic performance. Here we designed "negatively charged Ag (nc-Ag)" active sites featuring both the intrinsic activity and the capability of regulating microenvironment, through modifying Ag nanoparticles with atomically dispersed Sn species. Different from conventional active sites (which only mediate the surface processes by bonding with the intermediates), the nc-Ag sites could also manipulate environmental species. Therefore, the sites could not only activate CO2, but also regulate interfacial H2O and CO2, as confirmed by operando spectroscopies. The catalyst delivers a high current density with a CO faradaic efficiency of 97 %. Our work here opens up new opportunities for the design of multifunctional electrocatalytic active sites.
Keyword ：
CO2 electro-reduction CO2 electro-reduction Microenvironment manipulation Microenvironment manipulation Multifunctional active sites Multifunctional active sites nanocatalyst nanocatalyst
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| GB/T 7714 | Dai, Ruoyun , Sun, Kaian , Shen, Rongan et al. Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (37) . |
| MLA | Dai, Ruoyun et al. "Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 37 (2024) . |
| APA | Dai, Ruoyun , Sun, Kaian , Shen, Rongan , Fang, Jinjie , Cheong, Weng-Chon , Zhuang, Zewen et al. Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (37) . |
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Abstract ：
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.
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| GB/T 7714 | Wang, Kaili , Pei, Maojun , Shuai, Yankang 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, Kaili et al. "Rapid Two Surface Reconstructions of Ni/MnO Heterojunction for Superior Urea Electrolysis" . | ACS ENERGY LETTERS 9 . 9 (2024) : 4682-4690 . |
| APA | Wang, Kaili , Pei, Maojun , Shuai, Yankang , Liu, Yao , Deng, Shuqi , Zhuang, Zewen 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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