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Oxygen reduction electrocatalysis:From conventional to single-atomic platinum-based catalysts for proton exchange membrane fuel cells

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Frontiers in energy 2024年第2期18卷 206-222页

作者： Cheng YUAN Shiming ZHANG Jiujun ZHANG institute for sustainable energy/college of sciences Shanghai UniversityShanghai 200444China

Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction.Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts,Pt single-atom catalysts(Pt SACs)as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper.The design thoughts and synthesis of various isolated,alloyed,and nanoparticlecontained Pt SACs are summarized.The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts.To advance further research and development of Pt SACs for viable implementation in PEMFCs,various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis Pt singleatom catalysts conventional Pt-based catalysts design thoughts and synthesis metal-support interactions

Electron engineering of nickel phosphide for Ni^(δ+) in electrochemical nitrate reduction to ammonia

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Nano Research 2024年第6期17卷 4864-4871页

作者： Jie Hu Hao Huang Miao Yu Shuang Wang Jinping Li college of Environmental science and Engineering Taiyuan University of TechnologyJinzhong 030600China School of sustainable energy Materials and science Jinhua Advanced Research InstituteJinhua 321000China Shanxi Key Laboratory of Gas energy Efficient and Clean Utilization Taiyuan University of TechnologyTaiyuan 030024China

The electrochemical reduction of nitrate to ammonia(ENRA)provides an efficient approach to remove nitrate pollution and achieve ammonia production simultaneously.Herein,inspired by bio-enzyme in denitrifying bacteria,a carbon-coated nickel phosphide(NiPC)nanosheet derived from metal-organic frameworks(MOFs)is proposed as an efficient catalyst for ENRA.Through electron engineering,controllable Ni^(δ+)in nickel phosphide is achieved by regulating the degree of phosphating,which enhances its activity for the hydrogenation of nitrate.As the result,Niδ+becomes one of dominating factors determining the efficiency of the ENRA reaction in nickel phosphide.The optimal NiPC catalyst exhibits impressive property toward ENRA:NH_(4)^(+)Faraday efficiency of 96.68%,NH4+selectivity of 99.04%,and nitrate conversion rate of 90.43%under low nitrate concentration(200 mg·L^(−1)).This work opens a new avenue for the design of next-generation catalysts through electron engineering for ENRA.

关键词： electron engineering transition metal phosphide nitrate reduction ammonia production metal-organic frameworks

Self assembled electron blocking and lithiophilic interface towards dendrite-free solid-state lithium battery

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Chinese Chemical Letters 2024年第4期35卷 220-225页

作者： Caixia Li Yi Qiu Yufeng Zhao Wuliang Feng institute for sustainable energy&college of sciences Shanghai UniversityShanghai 200444China Key Laboratory of Advanced energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer from.Reducing the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable Li I interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li_7La_(3)Zr_(2)O_(12)(LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I_(2) thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm^(2) to 57 Ω/cm^(2). More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the Li I interphase, which leaded to a high critical current density of 1.2/7.0 m A/cm^(2) in the time/capacity-constant modes, respectively.

关键词： Li_7La_(3)Zr_(2)O_(12) LiI interphase Interfacial contact Li dendrite Thermodynamic stable

Model reduction of fractional impedance spectra for time–frequency analysis of batteries, fuel cells, and supercapacitors

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Carbon energy 2024年第1期6卷 108-141页

作者： Weiheng Li Qiu-An Huang Yuxuan Bai Jia Wang Linlin Wang Yuyu Liu Yufeng Zhao Xifei Li Jiujun Zhang institute for sustainable energy/college of sciences Shanghai UniversityShanghaiChina Shanxi Key Laboratory of Nanomaterials and Nanotechnology School of Mechanical and Electrical EngineeringXi'an University of Architecture and TechnologyXi'anShaanxiChina Xi'an Key Laboratory of New energy Materials and Devices School of Materials Science and EngineeringInstitute of Advanced Electrochemical EnergyXi'an University of TechnologyXi'anShaanxiChina

Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.

关键词： battery,fuel cell,supercapacitor fractional impedance spectroscopy model reduction time-frequency analysis

Fundamental Understanding of Hydrogen Evolution Reaction on Zinc Anode Surface:A First‑Principles Study

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Nano-Micro Letters 2024年第6期16卷 180-191页

作者： Xiaoyu Liu Yiming Guo Fanghua Ning Yuyu Liu Siqi Shi Qian Li Jiujun Zhang Shigang Lu Jin Yi institute for sustainable energy&Department of Chemistry Shanghai UniversityShanghai 200444People’s Republic of China School of Materials science and Engineering Shanghai UniversityShanghai 200444People’s Republic of China college of Materials science and Engineering National Engineering Research Center for Magnesium AlloysChongqing UniversityChongqing 400044People’s Republic of China

Hydrogen evolution reaction(HER)has become a key factor affecting the cycling stability of aqueous Zn-ion batteries,while the corresponding fundamental issues involving HER are still unclear.Herein,the reaction mechanisms of HER on various crystalline surfaces have been investigated by first-principle calculations based on density functional theory.It is found that the Volmer step is the ratelimiting step of HER on the Zn(002)and(100)surfaces,while,the reaction rates of HER on the Zn(101),(102)and(103)surfaces are determined by the Tafel step.Moreover,the correlation between HER activity and the generalized coordination number(CN)of Zn at the surfaces has been revealed.The relatively weaker HER activity on Zn(002)surface can be attributed to the higher CN of surface Zn atom.The atomically uneven Zn(002)surface shows significantly higher HER activity than the flat Zn(002)surface as the CN of the surface Zn atom is lowered.The CN of surface Zn atom is proposed as a key descriptor of HER activity.Tuning the CN of surface Zn atom would be a vital strategy to inhibit HER on the Zn anode surface based on the presented theoretical studies.Furthermore,this work provides a theoretical basis for the in-depth understanding of HER on the Zn surface.

关键词： Aqueous Zn-ion battery Zn anode Hydrogen evolution reaction Coordination number First-principles calculation

MOF-derived porous graphitic carbon with optimized plateau capacity and rate capability for high performance lithium-ion capacitors

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International Journal of Minerals,Metallurgy and Materials 2024年第2期31卷 395-404页

作者： Ge Chu Chaohui Wang Zhewei Yang Lin Qin Xin Fan college of Materials science&Engineering Guilin University of TechnologyGuilin 541004China institute of energy Innovation College of Materials Science and EngineeringTaiyuan University of TechnologyTaiyuan 030024China

The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).

关键词： metal-organic framework porous graphitic carbon optimized plateau capacity kinetic analysis lithium-ion capacitor

Decouple charge transfer reactions in the Li-ion battery

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Journal of energy Chemistry 2024年第5期92卷 759-798页

作者： Yuxuan Bai Qiu-An Huang Kai Wu Jiujun Zhang institute for sustainable energy/college of sciences Shanghai UniversityShanghai 200444China Ningde Contemporary Innovation Laboratory Contemporary Amperex Technology Co.LimitedNingde 352100FujianChina

In the development of Li-ion batteries(LIBs)with high energy/power density,long cycle-life,fast charging,and high safety,an insight into charge transfer reactions is required.Although electrochemical impedance spectroscopy(EIS)is regarded as a powerful diagnosis tool,it is not a direct but an indirect measurement.With respect to this,some critical questions need to be answered:(i)why EIS can reflect the kinetics of charge transfer reactions;(ii)what the inherent logical relationship between impedance models under different physical scenes is;(iii)how charge transfer reactions compete with each other at multiple scales.This work aims at answering these questions via developing a theory framework so as to mitigate the blindness and uncertainty in unveiling charge transfer reactions in LIBs.To systematically answer the above questions,this article is organized into a three-in-one(review,tutorial,and research)type and the following contributions are made:(i)a brief review is given for impedance model development of the LIBs over the past half century;(ii)an open source code toolbox is developed based on the unified impedance model;(iii)the competive mechanisms of charge transfer reactions are unveiled based on the developed EIS-Toolbox@LIB.This work not only clarifies theoretical fundamentals,but also provides an easy-to-use open source code for EIS-Toolbox@LIB to optimize fast charge/discharge,mitigate cycle aging,and improve energy/power density.

关键词： Electrochemical impedance spectroscopy Unified impedance model Charge transfer reactions Solid/electrolyte diffusion Porous electrode EIS-Toolbox@LIB

Magnetic-biased chiral molecules enabling highly oriented photovoltaic perovskites

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National science Review 2024年第2期11卷 221-230页

作者： Jing Chen Caner Deger Zhen-Huang Su Kai-Li Wang Guang-Peng Zhu Jun-Jie Wu Bing-Chen He Chun-Hao Chen Tao Wang Xing-Yu Gao Ilhan Yavuz Yan-Hui Lou Zhao-Kui Wang Liang-Sheng Liao institute of Functional Nano&Soft Materials(FUNSOM) Laboratory of Advanced Negative Carbon TechnologiesSoochow University Department of Physics Marmara University Shanghai Synchrotron Radiation Facility(SSRF) Shanghai Advanced Research InstituteChinese Academy of Sciences college of energy Soochow Institute for Energy and Materials Innovations Soochow University Macao institute of Materials science and Engineering Macau University of Science and Technology

The interaction between sites A, B and X with passivation molecules is restricted when the conventional passivation strategy is applied in perovskite（ABX3） photovoltaics. Fortunately, the revolving A-site presents an opportunity to strengthen this interaction by utilizing an external field. Herein, we propose a novel approach to achieving an ordered magnetic dipole moment, which is regulated by a magnetic field via the coupling effect between the chiral passivation molecule and the A-site（formamidine ion） in perovskites.This strategy can increase the molecular interaction energy by approximately four times and ensure a well-ordered molecular arrangement. The quality of the deposited perovskite film is significantly optimized with inhibited nonradiative recombination. It manages to reduce the open-circuit voltage loss of photovoltaic devices to 360 mV and increase the power conversion efficiency to 25.22%. This finding provides a new insight into the exploration of A-sites in perovskites and offers a novel route to improving the device performance of perovskite photovoltaics.

关键词： perovskite photovoltaics magnetic moment A-site regulation chiral molecules

Imaging plate scanners calibration and the attenuation behavior of imaging plate signals

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Chinese Physics B 2024年第6期33卷 38-44页

作者：薄楠王乃彦 college of Nuclear science and Technology Beijing Normal UniversityBeijing 100875China China institute of Atomic energy Beijing 102413China

Based on previously reported work, we propose a new method for calibrating image plate(IP) scanners, offering greater flexibility and convenience, which can be extended to the calibration tasks of various scanner models. This method was applied to calibrate the sensitivity of a GE Typhoon FLA 7000 scanner. Additionally, we performed a calibration of the spontaneous signal attenuation behavior for BAS-MS, BAS-SR, and BAS-TR type IPs under the 20±1℃ environmental conditions, and observed significant signal carrier diffusion behavior in BAS-MS IP. The calibration results lay a foundation for further research on the interaction between ultra-short, ultra-intense lasers and matter.

关键词： image plate scanner ultra-short ultra-intense lasers