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Achieving asymmetric redox chemistry for oxygen evolution reaction through strong metal-support interactions

Journal of energy Chemistry 2024年第9期96卷 526-535页

作者： Shihao Wang Meiling Fan Hongfei Pan Jiahui Lyu Jinsong Wu Haolin Tang Haining Zhang State Key Laboratory of Advanced technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina National energy Key Laboratory for New hydrogen-Ammonia energy Technologies Foshan Xianhu LaboratoryFoshan 528200GuangdongChina International School of Materials Science and Engineering(School of Materials and Microelectronics) Wuhan University of TechnologyWuhan 430070HubeiChina Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070HubeiChina Hubei Key Laboratory of Fuel Cell Wuhan University of TechnologyWuhan 430070HubeiChina

Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)*** this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through ***^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for *** Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current *** approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.

关键词： Reaction redox chemistry Strong metal-support interactions Layered double hydroxides Electrocatalysts Water electrolysis

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Exploring the Core-shell Structure of BaTiO3-based Dielectric Ceramics Using Machine Learning Models and Interpretability Analysis

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Journal of wuhan university of technology(Materials Science) 2024年第3期39卷 561-569页

作者：孙家乐 XIONG Peifeng 郝华 LIU Hanxing State Key Laboratory of Advanced technology for Materials Synthesis and Processing School of Material Science and EngineeringInternational School of Material Science and EngineeringWuhan University of TechnologyWuhan 430070China Sanya Science and Education Innovation Park Wuhan University of TechnologySanya 572000China Foshan Xianhu Laboratory of the Advanced energy Science and technology guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China

A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their interpretability was analyzed by using Shapley additive explanations(SHAP).An F1-score changed from 0.8795 to 0.9310,accuracy from 0.8450 to 0.9070,precision from 0.8714 to 0.9000,recall from 0.8929 to 0.9643,and ROC/AUC value of 0.97±0.03 was achieved by the RF classification with the optimal set of features containing only 5 features,demonstrating the high accuracy of our model and its high *** the interpretability analysis of the model,it was found that the electronegativity,melting point,and sintering temperature of the dopant contribute highly to the formation of the core-shell structure,and based on these characteristics,specific ranges were delineated and twelve elements were finally obtained that met all the requirements,namely Si,Sc,Mn,Fe,Co,Ni,Pd,Er,Tm,Lu,Pa,and *** the process of exploring the structure of the core-shell,the doping elements can be effectively localized to be selected by choosing the range of features.

关键词： machine learning BaTiO_(3) core-shell structure random forest classifier

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Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst

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Journal of energy Chemistry 2024年第1期88卷 543-551,I0012页

作者： Yingshi Su Yonghui Cheng Zhen Li Yanjia Cui Caili Yang Ziyi Zhong Yibing Song Gongwei Wang Lin Zhuang College of Chemistry&Chemical Engineering and Key Laboratory for Preparation and Application of Ordered Structural Materials of guangdong Province Shantou UniversityShantou 515063GuangdongChina College of Chemistry and Molecular Sciences Hubei Key Lab of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina The institute for Advanced Studies Wuhan UniversityWuhan 430072HubeiChina Department of Chemistry Engineering Guangdong Technion-Israel Institute of Technology(GTIIT)Shantou 515063GuangdongChina Technion-Israel institute of technology(IIT) Haifa 32000Israel

Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode ***,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)***,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)*** found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product *** to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology ***,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance.

关键词： Nafion modifier CO_(2)reduction Cu nanoparticles In situ ATR-SEIRAS C_(2)product

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Simple electrode assembly engineering:Toward a multifunctional lead-acid battery

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Journal of energy Chemistry 2024年第9期96卷 536-543页

作者： Xiaojuan Cao Xiaoyu Yan Kai Zhao Le Ke Xiaoyi Jiang Lingjiao Li Ning Yan Key Laboratory of Artificial Micro-and Nano-Structures of Ministry of Education School of Physics and TechnologyWuhan UniversityWuhan 430072HubeiChina Shenzhen Research institute of wuhan university Shenzhen 518057GuangdongChina

Electrochemical energy storage is a promising technology for the integration of renewable ***-acid battery is perhaps among the most successful commercialized systems ever since thanks to its excellent cost-effectiveness and safety *** of 165 years of development,the low energy density as well as the coupled power and energy density scaling restrain its wider application in real *** address this challenge,we optimized the configuration of conventional Pb-acid battery to integrate two gas diffusion *** novel device can work as a Pb-air battery using ambient air,showing a peak power density of 183 mW cm^(−2),which was comparable with other state-of-the-art metal-O_(2)*** can also behave as a fuel cell,simultaneously converting H_(2)and air into electricity with a peak power density of 75 mW cm^(−2).Importantly,this device showed little performance degradation after 35 h of the longevity *** work shows the exciting potential of lead battery technology and demonstrates the importance of battery architecture optimization toward improved energy storage capacity.

关键词： Lead-acid battery Decoupled electrode reaction energy storage Discharge capacity Fuel cell

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Isotropic sintering shrinkage of 3D glass-ceramic nanolattices:backbone preforming and mechanical enhancement

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International Journal of Extreme Manufacturing 2024年第2期6卷 418-426页

作者： Nianyao Chai Yunfan Yue Xiangyu Chen Zhongle Zeng Sheng Li Xuewen Wang Center of Femtosecond Laser Manufacturing for Advanced Materials and Devices State Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan 430070People’s Republic of China National energy Key Laboratory for New hydrogen-Ammonia energy Technologies Foshan Xianhu LaboratoryFoshan 528000People’s Republic of China International School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070People’s Republic of China

There is a perpetual pursuit for free-form glasses and ceramics featuring outstanding mechanical properties as well as chemical and thermal *** is a promising idea to shape inorganic materials in three-dimensional(3D)forms to reduce their weight while maintaining high mechanical properties.A popular strategy for the preparation of 3D inorganic materials is to mold the organic–inorganic hybrid photoresists into 3D micro-and nano-structures and remove the organic components by subsequent ***,due to the discrete arrangement of inorganic components in the organic-inorganic hybrid photoresists,it remains a huge challenge to attain isotropic shrinkage during ***,we demonstrate the isotropic sintering shrinkage by forming the consecutive–Si–O–Si–O–Zr–O–inorganic backbone in photoresists and fabricating 3D glass–ceramic nanolattices with enhanced mechanical *** femtosecond(fs)laser is used in two-photon polymerization(TPP)to fabricate 3D green body *** subsequent sintering at 1000℃,high-quality 3D glass–ceramic microstructures can be obtained with perfectly intact and smooth ***-suit compression experiments and finite-element simulations reveal that octahedral-truss(oct-truss)lattices possess remarkable adeptness in bearing stress concentration and maintain the structural integrity to resist rod bending,indicating that this structure is a candidate for preparing lightweight and high stiffness glass–ceramic nanolattices.3D printing of such glasses and ceramics has significant implications in a number of industrial applications,including metamaterials,microelectromechanical systems,photonic crystals,and damage-tolerant lightweight materials.

关键词： 3D printing isotropic shrinkage femtosecond laser two-photon polymerization structural glass-ceramics

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Surface repair of wide-bandgap perovskites for high-performance all-perovskite tandem solar cells

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Journal of energy Chemistry 2024年第6期93卷 64-70,I0003页

作者： Xiaojing Lv Weisheng Li Jin Zhang Yujie Yang Xuefei Jia Yitong Ji Qianqian Lin Wenchao Huang Tongle Bu Zhiwei Ren Canglang Yao Fuzhi Huang Yi-Bing Cheng Jinhui Tong State Key Laboratory of Advanced technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina Key Lab of Artificial Micro-and Nano-Structures of Ministry of Education of China School of Physics and TechnologyWuhan UniversityWuhan 430072HubeiChina Department of Electrical and Electronic Engineering Photonics Research Institute(PRI)Research Institute for Intelligent Wearable Systems(iWEAR)The Hong Kong Polytechnic University999077Hong KongChina Laboratory of Advanced Materials Fudan UniversityShanghai 200438China Xianhu Laboratory of the Advanced energy Science and technology guangdong Laboratory Foshan 528200GuangdongChina

Wide-bandgap(WBG)perovskite solar cells(PSCs)play a fundamental role in perovskite-based tandem solar ***,the efficiency of WBG PSCs is limited by significant open-circuit voltage losses,which are primarily caused by surface *** this study,we present a novel method for modifying surfaces using the multifunctional S-ethylisothiourea hydrobromide(SEBr),which can passivate both Pb^(-1)and FA^(-1)terminated surfaces,Moreover,the SEBr upshifted the Fermi level at the perovskite interface,thereby promoting carrier *** proposed method was effective for both 1.67 and 1.77 eV WBG PSCs,achieving power conversion efficiencies(PCEs)of 22.47%and 19.90%,respectively,with V_(OC)values of 1.28 and 1.33 V,along with improved film and device *** this advancement,we were able to fabricate monolithic all-perovskite tandem solar cells with a champion PCE of 27.10%,This research offers valuable insights for passivating the surface trap states of WBG perovskite through rational multifunctional molecular engineering.

关键词： Wide-bandgap perovskite Surface defect Multifunctional molecule All-perovskite tandem solar cells

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Efficient flexible perovskite solar cells and modules using a stable SnO_(2)-nanocrystal isopropanol dispersion

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Nano Research 2024年第4期17卷 2704-2711页

作者： Zhiwei Su Jing Li Ruixuan Jiang Shujie Zhang Chengkai Jin Feng Ye Bingcan Ke Mengjun Zhou Jinhui Tong Hyesung Park Fuzhi Huang Yi-Bing Cheng Tongle Bu State Key Laboratory of Advanced technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China School of Material Science and Engineering Wuhan University of TechnologyWuhan 430070China Department of Materials Science and Engineering Graduate School of Semiconductor Materials and Devices EngineeringGraduate School of Carbon NeutralityLow Dimensional Carbon Materials CenterUlsan National Institute of Science and TechnologyUlsan 44919Republic of Korea Xianhu Laboratory of the Advanced energy Science and technology guangdong Laboratory Foshan 528200China

The outstanding advantages of lightweight and flexibility enable flexible perovskite solar cells(PSCs)to have great application potential in mobile energy *** to the low cost,low-temperature processibility,and high electron mobility,SnO_(2) nanocrystals have been widely employed as the electron transport layer in flexible *** prepare high-quality SnO_(2) layers,a monodispersed nanocrystal solution is normally ***,the SnO_(2) nanocrystals can easily aggregate,especially after long periods of ***,we develop a green and cost-effective strategy for the synthesis of high-quality SnO_(2) nanocrystals at low temperatures by introducing small molecules of glycerol,obtaining a stable and well-dispersed SnO_(2)-nanocrystal isopropanol dispersion *** to the enhanced dispersity and super wettability of this alcohol-based SnO_(2)-nanocrystal solution,large-area smooth and dense SnO_(2) films are easily deposited on the plastic conductive ***,this contributes to effective charge transfer and suppressed non-radiative recombination at the interface between the SnO_(2) and perovskite *** a result,a greatly enhanced power conversion efficiency(PCE)of 21.8%from 19.2%is achieved for small-area flexible PSCs.A large-area 5 cm×5 cm flexible perovskite solar mini-module with a champion PCE of 16.5%and good stability is also demonstrated via this glycerol-modified SnO_(2)-nanocrystal isopropanol dispersion approach.

关键词： tin oxide isopropanol dispersion colloid stability flexible perovskite solar cells

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In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

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Journal of energy Chemistry 2024年第1期88卷 282-292,I0007页

作者： Huanhui Chen Xing Cao Moujie Huang Xiangzhong Ren Yubin Zhao Liang Yu Ya Liu Liubiao Zhong Yejun Qiu Shenzhen Engineering Lab of Flexible Transparent Conductive Films School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina School of Resource and Environmental Sciences Wuhan UniversityWuhan 430072HubeiChina

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li ***,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state ***,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion *** the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li *** expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical *** Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 ***,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical *** present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

关键词： Solid-state lithium batteries Composite solid electrolyte In-situ polymerization Interfacial passivation layer Self-adaptability

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Insights into ionic association boosting water oxidation activity and dynamic stability

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Journal of energy Chemistry 2024年第2期89卷 99-109,I0004页

作者： Zanling Huang Shuqi Zhu Yuan Duan Chaoran Pi Xuming Zhang Abebe Reda Woldu Jing-Xin Jian Paul K.Chu Qing-Xiao Tong Liangsheng Hu Xiangdong Yao Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of guangdong Province Shantou UniversityShantou 515063GuangdongChina Chemistry and Chemical Engineering guangdong Laboratory Shantou 515063GuangdongChina State Key Laboratory of Refractories and Metallurgy and institute of Advanced Materials and Nanotechnology Wuhan University of Science and TechnologyWuhan 430081HubeiChina Department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongTat Chee AvenueKowloonHong KongChina School of Advanced energy Sun Yat-sen University(Shenzhen)Shenzhen 518107GuangdongChina

There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains ***,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of *** Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 *** results provide insights into the ioncatalyzed effects boosting OER performance.

关键词： Oxygen evolution reaction Fe(Ⅲ)-catalysis Ni-Fe binary active centers Ion-catalyzed effects Robust stability

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Improving discharge voltage and ion storage dynamic in polyaniline via modulation of carrier charge density for magnesiummetal batteries

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Nano Research 2024年第7期17卷 6168-6175页

作者： Ping Luo Feiyang Chao Chunli Zuo Wenwei Zhang Fangyu Xiong Zhen Huang Dongyao Zhu Gongtao Yu Wenhui Zhong Xingbao Chen Han Tang Xiujuan Wei Qinyou An Hubei Provincial Key Laboratory of Green Materials for Light Industry School of Materials and Chemical EngineeringHubei University of TechnologyWuhan 430068China State Key Laboratory of Advanced technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China College of Materials Science and Engineering Chongqing UniversityChongqing 400044China institute for Sustainable Transformation School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006China

Rechargeable magnesium-metal batteries(RMBs)have gained much attention due to their abundant resources as well as high ***,the high charge density of Mg^(2+)is one of the main reasons for the slow kinetics performance of RMBs,and modulation of the charge density is an important strategy to improve the kinetics and electrochemical performance of ***,we report on the conductive polymer polyaniline(PANI)for RMBs,which is found to have excellent kinetics and high discharge voltage when storing MgCl^(+).In the storage of MgCl^(+),PANI exhibits a high average discharge voltage platform is 2.3 V ***^(2+)/Mg,which is higher than that in storage of Mg^(2+).We demonstrated the reversible intercalation/de-intercalation of MgCl^(+)in PANI accompanying with the reversible transformation between the quinone ring(C–C,–N=)and the benzene ring(C=C,–NH–)during charging and *** functional theory calculation reveals that PANI exhibit higher voltages(2.25 V vs.1.82 V)along with lower diffusion energy barriers(1.27 eV vs.1.55 eV)for MgCl^(+)storage compared to Mg^(2+)*** work refines the storage mechanism of PANI in RMBs and provides new guidelines for the application of PANI in RMBs.

关键词： rechargeable magnesium-metal batteries cathode materials polyaniline MgCl+storage

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