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Concurrently Boosting Activity and Stability of oxygen reduction reaction Catalysts via Judiciously Crafting Fe-Mn Dual Atoms for Fuel Cells

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Nano-Micro Letters 2025年第4期17卷 275-289页

作者： Lei Zhang Yuchen Dong Lubing Li Yuchuan Shi Yan Zhang Liting Wei Chung-Li Dong Zhiqun Lin Jinzhan Su International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049People’s Republic of China Department of Physics Tamkang UniversityNew Taipei CityTaiwan 25137People’s Republic of China Department of Chemical and Biomolecular Engineering National University of SingaporeEngineering Drive 4Singapore 117585Singapore

The ability to unlock the interplay between the activity and stability of oxygen reduction reaction(ORR)represents an important endeavor toward creating robust ORR catalysts for efficient fuel ***,we report an effective strategy to concurrent enhance the activity and stability of ORR catalysts via constructing atomically dispersed Fe-Mn dualmetal sites on N-doped carbon(denoted(FeMn-DA)-N-C)for both anion-exchange membrane fuel cells(AEMFC)and proton exchange membrane fuel cells(PEMFC).The(FeMn-DA)-N-C catalysts possess ample dual-metal atoms consisting of adjacent Fe-N_(4)and Mn-N_(4)sites on the carbon surface,yielded via a facile doping-adsorption-pyrolysis *** introduction of Mn carries several advantageous attributes:increasing the number of active sites,effectively anchoring Fe due to effective electron transfer to Mn(revealed by X-ray absorption spectroscopy and density-functional theory(DFT),thus preventing the aggregation of Fe),and effectively circumventing the occurrence of Fenton reaction,thus reducing the consumption of ***(FeMn-DA)-N-C catalysts showcase half-wave potentials of 0.92 and 0.82 V in 0.1 M KOH and 0.1 M HClO_(4),respectively,as well as outstanding *** manifested by DFT calculations,the introduction of Mn affects the electronic structure of Fe,down-shifts the d-band Fe active center,accelerates the desorption of OH groups,and creates higher limiting *** AEMFC and PEMFC with(FeMn-DA)-N-C as the cathode catalyst display high power densities of 1060 and 746 mW cm^(-2),respectively,underscoring their promising potential for practical *** study highlights the robustness of designing Fe-containing dual-atom ORR catalysts to promote both activity and stability for energy conversion and storage materials and devices.

关键词： Doping-adsorption-pyrolysis Dual-atom catalysts oxygen reduction reaction Fuel cells

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Understanding amorphous PrO_(x)-based N-doped carbon catalyst as an efficient electrocatalyst for oxygen reduction reaction

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Journal of Rare Earths 2025年第1期43卷 73-80,I0003页

作者： Xiao Man Ying Chang Shaohong Guo Meilin Jia Jingchun Jia Inner Mongolia Key Laboratory of Green Catalysis and Inner Mongolia Collaborative Innovation Center for Water Environment Safety College of Chemistry and Environmental ScienceInner Mongolia Normal UniversityHohhot010022China

The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-based catalyst PrO_(x)-NC,and optimized the calcination temperature and *** PrO_(x)-NC-900 catalyst has high durability and activity and exhibits superior ORR performance in alkaline electrolytes with an onset potential(E_(0))of 0.96 V and a half-wave potential(E_(1/2))of 0.85 *** research results indicate that the ORR performance of rare earth oxide composite carbon catalysts can be improved by adjusting oxygen vacancies(Ov).In addition,high specific surface area,N rich defect *** oxygen vacancies,and the synergistic effect of oxygen vacancies and N-doped carbon interfacial layer play a significant part in the enhancement of *** performance of the zinc air battery assembled with PrO_(x)-NC-900 is significantly improved,and rare earth oxides and carbon frameworks originating from metal organic frameworks(MOFs)contribute to the oxygen electrocatalyst and electron transfer rate of the zinc air *** catalyst provides promising information for the development of rare earth metal oxide nanostructures as potential candidate materials for ORR in alkaline media.

关键词： Rare earths Metal-organic framework oxygen reduction reaction Zn-air batteries

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Regulating local electron transfer environment of covalent triazine frameworks through F,N co-modification towards optimized oxygen reduction reaction

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Chinese Chemical Letters 2025年第1期36卷 344-348页

作者： Quanyou Guo Yue Yang Tingting Hu Hongqi Chu Lijun Liao Xuepeng Wang Zhenzi Li Liping Guo Wei Zhou Shandong Provincial Key Laboratory of Molecular Engineering School of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Ji’nan 250353China

The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active ***,the electronic conductivity is a vital parameter for oxygen reduction reaction(ORR).Covalent triazine frameworks(CTFs)have shown great potential application as electrocatalysts in ORR with a merit of the diverse building ***,the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic ***,CTFs were constructed by introducing F and N co-modification for efficient 2e^(-)*** with the pristine CTF,the co-presence of F,N could increase the conductivity obviously by *** a result,F-N-CTF exhibits enhanced catalytic performance of H_(2)O_(2)generation and selectivity towards reaction *** work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e^(-)ORR.

关键词： Covalent triazine frameworks Conductivity Co-modification Electrocatalysis oxygen reduction reaction

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Interfacial Pt-N coordination for promoting oxygen reduction reaction

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Chinese Chemical Letters 2025年第2期36卷 509-513页

作者： Jialin Cai Yizhe Chen Ruiwen Zhang Cheng Yuan Zeyu Jin Yongting Chen Shiming Zhang Jiujun Zhang Institute for Sustainable Energy/College of Sciences Shanghai University School of Chemistry and Chemical Engineering Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials Wuhan University of Science and Technology

Nitrogen-doping of carbon support（N-C） for platinum（Pt） nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction（ORR）in proton exchange membrane fuel cells. For fundamental understanding, clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed. In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations. The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H2-O2fuel cell. Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles, which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.

关键词： N-doped carbon oxygen reduction reaction Platinum Pt-N Theoretical calculations

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De novo-design of highly exposed Co−N−C single-atom catalyst for oxygen reduction reaction

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燃料化学学报(中英文) 2025年第1期53卷 128-137页

作者： ZHOU Dan ZHU Hongyue ZHAO Yang LIU Yiming Shanxi Key Laboratory of Catalysis and Energy Coupling School of Chemical Engineering and TechnologyTaiyuan University of Science and TechnologyTaiyuan 030024China Dalian National Laboratory for Clean Energy(DNL) Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely ***,most of metal single atoms in these catalysts were buried in the carbon matrix,resulting in a low metal utilization and inaccessibility for adsorption of reactants during the catalytic ***,we reported a facile synthesis based on the hard-soft acid-base(HSAB)theory to fabricate Co single-atom catalysts with highly exposed metal atoms ligated to the external pyridinic-N sites of a nitrogen-doped carbon *** from the highly accessible Co active sites,the prepared Co−N−C SAC exhibited a superior oxygen reduction reactivity comparable to that of the commercial Pt/C catalyst,showing a high turnover frequency(TOF)of 0.93 e^(−)·s^(-1)·site^(-1)at 0.85 V ***,far exceeding those of some representative SACs with a ultra-high metal *** work provides a rational strategy to design and prepare M−N−C single-atom catalysts featured with high site-accessibility and site-density.

关键词： hard-soft acid-base Co−N−C single-atom catalyst highly accessible active sites oxygen reduction reaction

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Ligand engineering of Co-MOF-74 with hexaaminotriphenylene for enhanced oxygen reduction reaction in zinc-air batteries

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Nano Research 2025年第2期18卷 290-297页

作者： Wei Liu Yu Liang Mengtian Huo Nan Ma Kaichi Qin Jinfa Chang Zihao Xing Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

Zinc-air batteries hold great promise as a next-generation efficient and environmentally friendly energy ***,the sluggish kinetics of the oxygen reduction reaction(ORR)process pose a significant challenge to their *** address this issue,atom dispersion catalysts are developed to maximize the utilization of metal active ***-organic frameworks(MOFs)are a series of molecular materials with high atomic-level dispersion metal utilization,but they often lack sufficient electrical *** application in MOF electrocatalysis remains limited unless the MOF material is transferred to a carbon-based material through heat *** overcome this limitation,we employed coordination engineering to incorporate hexaaminotriphenylene(HATP)molecules with strong conjugation into *** resulting Co-MOF-74-HATP catalyst represents high activity,achieving an ORR half-wave potential(E_(1/2))of 0.84 V and demonstrating good stability(ΔE_(1/2)=20 mV after 10,000 cycles).Additionally,the Co-MOF-74-HATP also performs a 320 mV overpotential(10 mA·cm^(-2))for the oxygen evolution ***,Co-MOF-74-HATP displays a peak power density of 96.6 mW·cm^(-2) in zinc-air batteries,surpassing the commercially available Pt/C+RuO_(2).This work presents a new pathway to design MOF-based ORR catalysts and provides a new direction for the preparation of key materials for zinc-air battery(ZAB).

关键词： molecular catalysts oxygen reduction reaction zinc-air battery coordination environment metal-organic framework

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oxygen reduction reaction performance of Fe-N-C catalyst with dual nitrogen source

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Frontiers in Energy 2024年第6期18卷 841-849页

作者： Yuan Zhao Quan Wang Rongrong Hu Wenqiang Liu Xiaojuan Zhang Wei Wang Nicolas Alonso-Vante Dongdong Zhu School of Materials Engineering Jinling Institute of TechnologyNanjing 211169China School of Energy and Power Engineering Nanjing University of Science and TechnologyNanjing 210094China IC2MP UMR-CNRS 7285University of PoitiersF-86073 Poitiers CedexFrance Institute of Advanced Materials and Flexible Electronics School of Chemistry and Materials ScienceNanjing University of Information Science and TechnologyNanjing 210044China

Fe-N-C catalysts are potential substitutes to displace electrocatalysts containing noble chemical elements in the oxygen reduction reaction(ORR).However,their application is hampered by unsatisfactory activity and stability *** structures and morphologies of Fe-N-C catalysts have been found to be crucial for the number of active sites and local bonding *** this work,dicyandiamide(DCDA)and polyaniline(PANI)are shown to act as dual nitrogen sources to tune the morphology and structure of the catalyst and facilitate the ORR *** dual nitrogen sources not only increase the amount of nitrogen doping atoms in the electrocatalytic Fe-C-N material,but also maintain a high nitrogen-pyrrole/nitrogen-graphitic:(N-P)/(N-G)value,improving the distribution density of catalytic active sites in the *** a high surface area and amount of N-doping,the Fe-N-C catalyst developed can achieve an improved half-wave potential of 0.886 V(***)in alkaline medium,and a better stability and methanol resistance than commercial Pt/C catalyst.

关键词： Fe-N-C oxygen reduction reaction nitrogen-doped dual nitrogen source

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oxygen reduction reaction on single Pt nanoparticle

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Journal of Energy Chemistry 2020年第10期29卷 323-326页

作者： Zhi-Peng Xiang Ai-Dong Tan Zhi-Yong Fu Jin-Hua Piao Zhen-Xing Liang Key Laboratory on Fuel Cell Technology of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641GuangdongChina School of Food Science and Engineering South China University of TechnologyGuangzhou 510641GuangdongChina

Nanocollision electrochemistry is employed to evaluate the ORR’s activity of one single Pt nanoparticle,the effect of the size and ligand is *** size-normalized activity of the Pt nanoparticle of 4 nm is two times higher than that of 25 nm,confirming that the intrinsic activity does depend on the size of the *** is further found that the adsorbed ligand does yield effect on electrocatalysis,and the adsorption strength follows the order of PVP>CTAB>*** work is of significance to understand the nature of the ORR’s electrocatalysis at the level of an individual entity,which makes the structure-activity correlation in a more reliable way.

关键词： Ligand effect Nano-collision electrochemistry oxygen reduction reaction Single Pt nanoparticle

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Pyrolysis of Copper Phthalocyanine as Non-noble Metal Electrocatalysts for oxygen reduction reaction

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Journal of Wuhan University of Technology(Materials Science) 2024年第5期39卷 1087-1092页

作者： ZHANG Lijuan LU Jinhua WANG Yan LI Xiang School of Materials and Chemical Engineering Xi’an Technological UniversityXi’an 710021China State Key Laboratory of Solidification Processing Carbon/Carbon Composites Research CenterNorthwestern Polytechnical UniversityXi’an710072China

We investigated the relationship between oxygen reduction reaction(ORR)activity and the pyrolysis temperature(650-850℃)of CuPc in alkaline *** highly active sites were formed through the decomposition of CuPc or Cu-N_(4) structure after releasing ***-Nx incorporated with carbon were the main active *** XPS measurement results show that,at lower temperature,the contents of pyridinic-N and pyrrolic-N account for the most of the total *** the temperature is higher than 750℃,the content of graphitic N(26.11%)increases and pyridinic-N(58.81%)becomes the dominant *** the temperature is higher than 850℃,the content of graphitic N increases remarkably and becomes the dominant ***,the specific surface areas decrease with increased pyrolysis *** from the synergistic effect,the pyrolysis temperature at 750℃of CuPc displays superior electrocatalytic *** obtained results reveal that the fabricated non-noble metal catalysts can be used as low-cost,efficient catalyst for water splitting ORR in metal-air batteries and fuel cells.

关键词： copper phthalocyanine pyrolysis electrocatalytic oxygen reduction reaction

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Ultrastable bimetallic Fe_(2)Mo for efficient oxygen reduction reaction in pH-universal applications

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Nano Research 2022年第6期15卷 4950-4957页

作者： Jue Hu Chengxu Zhang Mingzi Sun Qianglong Qi Shanxiong Luo Hongchuan Song Jingyi Xiao Bolong Huang Michael K.H.Leung Yingjie Zhang The Engineering Laboratory of Advanced Battery and Materials of Yunnan Province Kunming University of Science and TechnologyKunming 650093China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina School of Energy and Environment Science Yunnan Normal UniversityKunming 650500China Ability R&D Energy Research Centre School of Energy and EnvironmentCity University of Hong KongHong KongChina

Iron-based nanostructures represent an emerging class of catalysts with high electroactivity for oxygen reduction reaction(ORR)in energy storage and conversion ***,current practical applications have been limited by insufficient durability in both alkaline and acidic *** particular,limited attention has been paid to stabilizing iron-based catalysts by introducing additional metal by the alloying ***,we report bimetallic Fe_(2)Mo nanoparticles on N-doped carbon(Fe_(2)Mo/NC)as an efficient and ultra-stable ORR electrocatalyst for the first *** Fe_(2)Mo/NC catalyst shows high selectivity for a four-electron pathway of ORR and remarkable electrocatalytic activity with high kinetics current density and half-wave potential as well as low Tafel slope in both acidic and alkaline *** demonstrates excellent long-term durability with no activity loss even after 10,000 potential *** functional theory(DFT)calculations have confirmed the modulated electronic structure of formed Fe_(2)Mo,which supports the electron-rich structure for the ORR ***,the mutual protection between Fe and Mo sites guarantees efficient electron transfer and long-term stability,especially under the alkaline *** work has supplied an effective strategy to solve the dilemma between high electroactivity and long-term durability for the Fe-based electrocatalysts,which opens a new direction of developing novel electrocatalyst systems for future research.

关键词： oxygen reduction reaction Fe2Mo bimetallic nanoparticles zeolitic imidazolate frameworks(ZIFs) ultralong stability superior oxygen reduction reaction(ORR)performance

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