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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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The oxygen reduction reaction (ORR) is critical for energy conversion technologies like fuel cells and metal-air batteries. However, advancing efficient and stable ORR catalysts remains a significant challenge. Iron-based single-atom catalysts (Fe SACs) have emerged as promising alternatives to precious metals. However, their catalytic performance and stability remain constrained. Introducing a second metal (M) to construct Fe & horbar;M dual-atom catalysts (Fe & horbar;M DACs) is an effective strategy to enhance the performance of Fe SACs. This review provides a comprehensive overview of the recent advancements in Fe-based DACs for ORR. It begins by examining the structural advantages of Fe & horbar;M DACs from the perspectives of electronic structure and reaction pathways. Next, the precise synthetic strategies for DACs are discussed, and the structure-performance relationships are explored, highlighting the role of the second metal in improving catalytic activity and stability. The review also covers in situ characterization techniques for real-time observation of catalytic dynamics and reaction intermediates. Finally, future directions for Fe & horbar;M DACs are proposed, emphasizing the integration of advanced experimental strategies with theoretical simulations as well as artificial intelligence/machine learning to design highly active and stable ORR catalysts, aiming to expand the application of Fe & horbar;M DACs in energy conversion and storage technologies.
Keyword ：
dual-atom catalysts dual-atom catalysts iron-based electrocatalysts iron-based electrocatalysts oxygen reduction reaction oxygen reduction reaction single-atom catalyst single-atom catalyst
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| GB/T 7714 | You, Shengping , Zhang, Chao , Yu, Mingyu et al. Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts [J]. | SMALL , 2025 , 21 (27) . |
| MLA | You, Shengping et al. "Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts" . | SMALL 21 . 27 (2025) . |
| APA | You, Shengping , Zhang, Chao , Yu, Mingyu , Tan, Xin , Sun, Kaian , Zheng, Yun et al. Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts . | SMALL , 2025 , 21 (27) . |
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The carbon dioxide electroreduction reaction (CO2RR) to ethanol (C2H5OH) represents a sustainable route toward carbon neutrality. Herein, we present the design of enzyme-inspired zirconium-Fe porphyrinic-based metal-organic framework (MOF) nanosheets functionalized with 5-benzimidazolecarboxylic acid (FeTCPP-NSs-BAA) for the CO2RR. Electrochemical performances in a H-cell reveal that FeTCPP-NSs-BAA shows C2H5OH faradaic efficiencies (FEs) of 79.8% under neutral and 89.2% under acidic conditions, with C2H5OH FEs exceeding 60% over wide potential windows of -0.3 to -0.6 V and -0.3 to -0.8 V, respectively. In flow cell tests under acidic conditions, FeTCPP-NSs-BAA delivers the highest C2H5OH partial current density of 8.1 mA cm-2 with pure CO2, and a C2H5OH partial current density of 5.6 mA cm-2 when using 30% low-concentration CO2. In situ spectroscopic characterization and theoretical calculations reveal that the superior C2H5OH performance of FeTCPP-NSs-BAA arises from the enzyme-like non-covalent synergistic effects between FeTCPP and the secondary-sphere functionalities of BAA and Zr6 clusters. Specifically, BAA enhances CO2 enrichment and facilitates the tilted *CO adsorption at Fe centers on FeTCPP, which significantly reduces energy barriers for *CO-CO coupling compared to linearly adsorbed *CO. Meanwhile, the subsequent hydrogenation of *CO-CO to C2H5OH can be further accelerated by proton shuttling mediated through hydrogen-bonding networks introduced by Zr6 clusters.
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| GB/T 7714 | Sun, Kaian , Xie, Shaohui , Guan, Ping et al. A bioinspired electrocatalyst for CO2 electroreduction to ethanol via secondary-sphere synergy in Fe porphyrinic-based metal-organic frameworks [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (13) : 6823-6831 . |
| MLA | Sun, Kaian et al. "A bioinspired electrocatalyst for CO2 electroreduction to ethanol via secondary-sphere synergy in Fe porphyrinic-based metal-organic frameworks" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 13 (2025) : 6823-6831 . |
| APA | Sun, Kaian , Xie, Shaohui , Guan, Ping , Zhuang, Zewen , Tan, Xin , Yan, Wei et al. A bioinspired electrocatalyst for CO2 electroreduction to ethanol via secondary-sphere synergy in Fe porphyrinic-based metal-organic frameworks . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (13) , 6823-6831 . |
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Single-atomic/cluster metal-based electrocatalysts (M-N-C) is one of the most promising non-noble metal catalysts for the oxygen reduction reaction (ORR), but their practical application is severely hindered by insufficient activity and durability. Herein, charge regulation through rare earth metal oxides (REMOs) for single-atomic/cluster metal based electrocatalysts is proposed for boosting ORR, in which the Co-based catalyst is taken as a representative considering its typicality and universality, and CeO2 is selected as representative after systematic computational screening from more than 10 types of REMOs. As a result, a novel REMO-tailored M-N-C electrocatalyst (REMO-Co-N-C) has been successfully achieved, which demonstrates a remarkably increased activity and superior durability, namely a half-wave potential (E₁/₂) of 0.90 V and only a loss of 8 mV (E₁/₂) after 10,000 cycles. Moreover, in-situ experiments and matched theoretical simulations come together organically to clearly and directly reveal the origin and catalytic behavior of the proposed electrocatalysts. Namely the charge regulation through REMO for M-N-C can effectively modify the electronic structure of the M sites, accelerate the reaction rate, and enhance OH* desorption. This work offers a new insight for promoting M-N-C catalysts through REMO tailoring, that beyond the conventional use of d-block and p-block elements. © 2025 Elsevier B.V.
Keyword ：
Cerium oxide Cerium oxide Electrolysis Electrolysis Electrolytic reduction Electrolytic reduction
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| GB/T 7714 | Wang, Shufan , Li, Lingfei , Zheng, Yun et al. Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction [J]. | Applied Catalysis B: Environmental , 2025 , 377 . |
| MLA | Wang, Shufan et al. "Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction" . | Applied Catalysis B: Environmental 377 (2025) . |
| APA | Wang, Shufan , Li, Lingfei , Zheng, Yun , Xu, Chenhui , Zhuang, Zewen , Sun, Kaian et al. Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction . | Applied Catalysis B: Environmental , 2025 , 377 . |
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The electrochemical CO2 reduction reaction (CO2RR) provides a promising approach to mitigate the global greenhouse effect by converting CO2 into high-value chemicals or fuels. Noble metal-based nanomaterials are widely regarded as efficient catalysts for CO2RR due to their high catalytic activity and excellent stability. However, these catalysts typically favor the formation of C1 products, which have relatively low economic value. Moreover, the high cost and limited availability of noble materials necessitate strategies to reduce their usage, often by dispersing them on suitable support materials to enhance catalytic performance. In this study, a novel metal-based support, zirconium phosphate Zr-3(PO4)(4), was used to anchor ultrasmall palladium nanoparticles (pre-ZrP-Pd). Compared to the reversible hydrogen electrode, the pre-ZrP-Pd achieved a maximum Faradaic efficiency (FE) of 92.1% for ethanol at -0.8 V versus RHE, along with a peak ethanol current density of 0.82 mA/cm(2). Density functional theory (DFT) calculations revealed that the strong metal-support interactions between the ZrP support and Pd nanoparticles lead to an upward shift of the Pd d-band center, enhancing the adsorption of CO* and promoting the coupling of CO and CO to produce ethanol.
Keyword ：
density functional theory (DFT) calculations density functional theory (DFT) calculations electrochemical CO2 reduction reaction (CO2RR) electrochemical CO2 reduction reaction (CO2RR) ethanol selectivity ethanol selectivity noble metal-based nanocatalysts noble metal-based nanocatalysts zirconium phosphate (Zr-3(PO4)(4)) support zirconium phosphate (Zr-3(PO4)(4)) support
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| GB/T 7714 | Zhong, Bowen , Hu, Chengwei , Sun, Kaian et al. Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol [J]. | FRONTIERS IN ENERGY , 2025 , 19 (4) : 545-551 . |
| MLA | Zhong, Bowen et al. "Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol" . | FRONTIERS IN ENERGY 19 . 4 (2025) : 545-551 . |
| APA | Zhong, Bowen , Hu, Chengwei , Sun, Kaian , Yan, Wei , Zhang, Jiujun , Xie, Zailai . Ultrasmall palladium nanoparticles supported on zirconium phosphate for electrochemical CO2 reduction to ethanol . | FRONTIERS IN ENERGY , 2025 , 19 (4) , 545-551 . |
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Electrocatalytic nitrate reduction (NO3-RR) holds significant potential for clean NH3 synthesis and the treatment of industrial effluents, effectively converting waste into a valuable resource. However, the catalyst reconstruction mechanism remains ambiguous, and the influence of interfacial hydrogen bonds on NO3-RR performance remains underexplored. Herein, a Cr-doping strategy was developed to regulate the interfacial hydrogen-bonded interactions on Co-based dynamic electrocatalysts to improve electrocatalytic NO3-RR activity. In situ XRD, in situ Raman spectroscopy and theoretical calculations indicated that Cr doping could modulate the reconstruction process of Co-based materials, achieving a dynamic balance between Co(OH)2 and Co. Moreover, molecular dynamics simulations and density functional theory calculations, combined with in situ infrared spectroscopy, revealed that the strong hydrogen-bonding interactions between interfacial H2O and the Cr-doped Co(OH)2 surface could drag more free H2O from the rigid H2O network and facilitate H2O dissociation, forming active hydrogen to accelerate the NO3-RR pathway on metallic Co sites. As a result, the Cr-doped Co-based dynamic electrocatalyst displayed a superior NH3 faradaic efficiency of 97.36% and a high NH3 yield rate of 58.92 mg h-1 cm-2, outperforming the state-of-the-art electrocatalysts. This work can further inspire the design of dynamic electrocatalysts and the modulation of the interfacial microenvironment for promoting effective electrochemical hydrogenation reactions.
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| GB/T 7714 | Wan, Yuchi , Tang, Yixiang , Zuo, Yinze et al. Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) : 7460-7469 . |
| MLA | Wan, Yuchi et al. "Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 15 (2025) : 7460-7469 . |
| APA | Wan, Yuchi , Tang, Yixiang , Zuo, Yinze , Sun, Kaian , Zhuang, Zewen , Zheng, Yun et al. Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) , 7460-7469 . |
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| GB/T 7714 | Zhuang, Z. , Sun, K. , Zheng, Y. et al. Electrochemical CO2 reduction for reducing CO2 emission and producing value-added products [未知]. |
| MLA | Zhuang, Z. et al. "Electrochemical CO2 reduction for reducing CO2 emission and producing value-added products" [未知]. |
| APA | Zhuang, Z. , Sun, K. , Zheng, Y. , Yan, W. , Zhang, J. . Electrochemical CO2 reduction for reducing CO2 emission and producing value-added products [未知]. |
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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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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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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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