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Defects and morphology engineering for constructing V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S nanotube heterojunction arrays toward efficient bifunctional electrocatalyst for overall water splitting

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Journal of Energy Chemistry 2024年第7期94卷 29-40页

作者： Wenyuan Sun Alan Meng Lei Wang Guicun Li Jinfeng Cui Yongkai Sun Zhenjiang Li College of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Optic-electric Sensing and Analytical Chemistryfor Life science MOE College of Chemistry and Molecular EngineeringQingdao Universityof Science and TechnologyQingdao 266042ShandongChina College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Qingdao Huanghai University Qingdao 266000ShandongChina College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061ShandongChina

The development of highly active,stable and inexpensive electrocatalysts for hydrogen production by defects and morphology engineering remains a great ***,S vacancies-rich Ni_(3)S_(2)@Cu_(2)S nan-otube heterojunction arrays were in-situ grown on copper foam(V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF)for efficient electrocatalytic overall water *** the merits of nanotube arrays and efficient electronic mod-ulation drived by the OD vacancy defect and 2D heterojunction defect,the resultant V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF electrocatalyst exhibits excellent electrocatalytic activity with a low overpotential of 47 mV for the hydrogen evolution reaction(HER)at 10 mA cm^(-2) current density,and 263 mV for the oxygen evolution reaction(OER)at 50 mA cm^(-2) current density,as well as a cell voltage of 1.48 V at 10 mA cm^(-2).Moreover,the nanotube heterojunction arrays endows V_(s)-Ni_(3)S_(2)@V_(s)-Cu_(2)S NHAs/CF with outstanding stability in long-term catalytic processes,as confirmed by the continuous chronopotentiom-etry tests at current densities of 10 mA cm^(-2) for 100 h.

关键词： Nanotubearrays Heterojunction Vacancy Bifunctional electrocatalyst Overall water splitting

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Stable multi-electron reaction stimulated by W doping VS_(4)for enhancing magnesium storage performance

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Journal of Energy Chemistry 2024年第2期89卷 89-98,I0004页

作者： Yuxin Tian Jiankang Chen Guofeng Wang Bing Sun Alan Meng Lei Wang Guicun Li Jianfeng Huang Shiqi Ding Zhenjiang Li College of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life science MOEShandong Key Laboratory of Biochemical AnalysisCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina School of Material science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi’an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi’an 710021ShaanxiChina

Rechargeable magnesium batteries(RMBs)hold promise for offering higher volumetric energy density and safety features,attracting increasing research interest as the next post lithium-ion *** high performance cathode material by inducing multi-electron reaction process as well as maintaining structural stability is the key to the development and application of ***,multielectron reaction occurred in VS_(4)by simple W doping strategy.W doping induces valence of partial V as V^(2+)and V^(3+)in VS_(4)structure,and then stimulates electrochemical reaction involving multi-electrons in 0.5%*** flower-like microsphere morphology as well as rich S vacancies is also modulated by W doping to neutralize structure change in such multi-electron reaction *** fabricated 0.5%W-V-S delivers higher specific capacity(149.3 m A h g^(-1)at 50 m A g^(-1),which is 1.6 times higher than that of VS_(4)),superior rate capability(76 mA h g^(-1)at 1000 mA g^(-1)),and stable cycling performance(1500cycles with capacity retention ratio of 93.8%).Besides that,pesudocapaticance-like contribution analysis as well as galvanostatic intermittent titration technique(GITT)further confirms the enhanced Mg^(2+)storage kinetics during such multi-electron involved electrochemical reaction *** discovery provides new insights into the designing of multi-electron reaction process in cathode as well as neutralizing structural change during such reaction for realizing superior electrochemical performance in energy storage devices.

关键词： Multi-electron reaction W doping Stable structure Cathode Rechargeable magnesium batteries

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Bifunctional core–shell co-catalyst for boosting photocatalytic CO_(2) reduction to CH_(4)

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Nano research 2024年第3期17卷 1259-1266页

作者： Fangxu Dai Mingming Zhang Jishu Han Zhenjiang Li Shouhua Feng Jun Xing Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Solar-light-driven CO_(2) reduction CO to CH_(4) and C2H6 is a complex process involving multiple elementary reactions and energy ***,achieving high CH_(4) activity and selectivity remains a significant ***,we integrate bifunctional Cu2O and Cu-MOF(MOF=metal-organic framework)core–shell co-catalysts(Cu2O@Cu-MOF)with semiconductor TiO_(2).Experiments and theoretical calculations demonstrate that Cu2O(Cu+facilitates charge separation)and Cu-MOF(Cu2+improves the CO_(2) adsorption and activation)in the core–shell structure have a synergistic effect on photocatalytic CO_(2) reduction,reducing the formation barrier of the key intermediate*COOH and**** photocatalyst exhibits high CH_(4) yield(366.0μmol·g^(-1)·h^(-1)),efficient electron transfer(3283μmol·g^(-1)·h^(-1))and hydrocarbon selectivity(95.5%),which represents the highest activity of Cu-MOF-based catalysts in photocatalytic CO_(2) reduction *** work provides a strategy for designing efficient photocatalysts from the perspective of precise regulation of components.

关键词： bifunctional co-catalyst core–shell photocatalytic CO_(2)reduction

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Regulate electric double layer for one-step synthesize and modulate the morphology of(oxy)hydroxides

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Nano research 2024年第5期17卷 3675-3683页

作者： Jiaxin Liu Yue Shi Yanli Gu Zheng Lv Liang Zhao Yu Yang Tianrong Zhan Jianping Lai Lei Wang State Key Laboratory Base of Eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China shandong Engineering research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

FeOOH have received considerable attention due to their natural abundance and *** the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major ***,the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling ***,density functional theory(DFT)calculations and X-ray photoelectron spectroscopy(XPS)demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH,which further promotes the formation and stabilization of *** used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer(EDL)composition and *** prepared Co-FeOOH-K^(+)has a larger electrochemically active surface area(ECSA)(325 cm^(2))and turnover frequency(TOF)value(0.75 s^(-1)).In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer,Co-FeOOH-K^(+)shows better oxygen evolution performance than commercial RuO_(2) under industrial production conditions and has good industrial application prospects.

关键词： integrated(oxy)hydroxides electrodeposition electric double layer(EDL) oxygen evolution reaction(OER) morphology regulation

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Polysulfide modified PtCu intermetallic nanocatalyst with enrichment realizes efficient electrooxidation ethanol to CO_(2)

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Nano research 2024年第4期17卷 2320-2327页

作者： Shuanglong Zhou Zheng Lv Liang Zhao Dan Zhang Zuocao Wang Yu Dai Bin Li Olga Starostenko Jianping Lai Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationTaishan scholar advantage and characteristic discipline team of Eco-chemical process and technologyLaboratory of Inorganic Synthesis and Applied ChemistryCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Foreign Languages Qingdao City UniversityQingdao 266106China College of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042China Institute of Macromolecular Chemistry of the National Academy of sciences of Ukraine Kyiv 02160Ukraine shandong Engineering research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

The main problem faced by ethanol oxidation reaction(EOR)includes low activity,poor selectivity,and *** the study,we found that polysulfide modified on the surface of PtCu intermetallic(IM)/C can simultaneously enrich hydroxyl and ethanol,which could effectively improve the catalytic activity,CO_(2) selectivity,and durability of *** mass activity and the specific activity of the product in 1 M KOH electrolyte reached 17.83 A·mgPt^(-1) and 24.67 mA·cm^(-2).The CO_(2) selectivity of polysulfide modified product achieved 93.5%,which was 30 folds higher than Pt/*** addition,the catalyst showed high catalytic *** mechanism study demonstrates that the surface modified polysulfide could significantly boost the enrichment effect of ethanol and hydroxyl species,accelerating C–C bond cleavage and CO oxidation.

关键词： Pt CO_(2) selectivity enrichment effect ethanol oxidation reaction(EOR) electrocatalyst

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Acidic electroreduction CO_(2)to formic acid via interfacial modification of Bi nanoparticles at industrial-level current

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Nano research 2024年第7期17卷 5817-5825页

作者： Tian Dong Hongdong Li Zhenhui Wang Yanling Geng Rui Chang Xiaofeng Tian Jianping Lai Shouhua Feng Lei Wang Key Laboratory of Eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China shandong Engineering research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral ***,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current ***,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles *** a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FEHCOOH(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 *** with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.

关键词： acidic media CO_(2)electrolysis electrolyte additive hydrophobic interfacial microenvironment industrial-level current

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Hierarchical Fe_(x)Bi_(2−x)S_(3) solid solutions for boosted supercapacitor performance

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Nano research 2024年第5期17卷 3997-4005页

作者： Fengming Zhou Xiaodong Wang Ruijie Jing Xiaoyu Li Qi Zhang Zhenjiang Li Yunmei Du Zhenyu Xiao Lei Wang International Cooperation United Laboratory of Eco-chemical Engineering and Green Manufacturing College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Technology Innovation Center of Battery Safety and Energy Storage Technology QingdaoInternational Science and Technology Cooperation Base of QingdaoCollege of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

For the pursuit of high energy supercapacitors,the development of high performance pseudocapacitance or battery-type negative electrode material is urgently needed to make up for the capacity shortage of commercial electric double layer capacitor(EDLC)type ***,a porous and defect-rich Fe_(x)Bi_(2-x)S_(3) solid solution structure is firstly constructed by employing Fe-doped Bi_(2)O_(2)CO_(3) porous nanosheets as a precursor,which presents dramatically increased energy storage performance than Bi_(2)S_(3) and FeS_(2) *** the optimized Fe_(x)Bi_(2-x)S_(3) solid solution(FeBiS-60%),the Fe solute is free and random dispersed in Bi_(2)S_(3) framework,which can effectively modulate the electronic structure of Bi element and introduce rich-defect due to the existence of Fe(II).Meanwhile,the FeBiS-60%,constructed by pore nanosheets that are assembled by self-supported basic nanorod units,presents rich mesoporous channels for fast mass transfer and abundant active sites for promoting capacity ***,a high capacitance of 832.8 F·g^(-1) at a current density of 1 A·g^(-1) is achieved by the FeBiS-60%***,a fabricated Ni3S_(2)@Co_(3)S_(4)(NCS)//FeBiS-60%hybrid supercapacitor device delivers an outstanding energy density of 85.33 Wh·kg^(-1) at the power density of 0.799 kW·kg^(-1),and ultra-long lifespan of remaining 86.7%initial capacitance after 8700 cycles.

关键词： supercapacitor solid solutions defect structure hierarchical structure Bi_(2)S_(3)

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Surface/Interface Engineering of Hierarchical MoO_(2)/MoNi_(4)@Ru/RuO_(2)Heterogeneous Nanosheet Arrays for Alkaline Water Electrolysis with Fast Kinetics

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Chinese Journal of Chemistry 2024年第2期42卷 119-128页

作者： Qiong Zhang Ruixue Zhang Yingxiu Zhao Tiantian Sun Jianyang Gao Guang-Rui Xu Zexing Wu Yu Yang Lei Wang Key Laboratory of Eco-chemical Engineering Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life ScienceTaishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyCollege of Chemistry and Molecular EngineeringSchool of Materials Science and EngineeringQingdao University of Science and TechnologyQingdaoShandong 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdaoShandong 266042China

Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water ***,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of *** from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)*** synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water ***,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline *** building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.

关键词： Hierarchical heterostructure Surface engineering Bifunctional catalysts Hydrogen evolution reaction Oxygen evolution reaction Watersplitting Catalytic activity Electrocatalysis Heterogeneous catalysis

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RuO_(2)/TiO_(2)/MXene with multi-heterojunctions coating on carbon cloth for high-activity chlorine evolution reaction at large current densities

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Nano research 2024年第6期17卷 4764-4772页

作者： Yuhao Duan Liuxu Wei Chenyu Cai Junbao Mi Fuyuan Cao Jiaze Chen Xiaolong Li Xiujiang Pang Bin Li Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationInternational Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China

The chlorine evolution reaction(CER)is a crucial step in the production of chlorine gas and active chlorine by chlor-alkali ***,the endeavor to fabricate electrodes capable of yielding high current density at minimal overpotential remains a central challenge in advancing the realm of chlorine evolution ***,we grow TiO_(2)and RuO_(2)on MXene@carbon cloth(CC)through the favorable affinity and induced deposition effect between the surface functional groups of MXene and the metal.A self-supported electrode(RuTiO_(2)/MXene@CC)with strong binding at the electrocatalyst-support interface and weak adhesion at electrocatalyst-bubble interface is *** RuTiO_(2)/MXene@CC can reduce the electron density of RuO_(2)by regulating the electron redistribution at the heterogeneous interface,thus enhancing the adsorption of Cl−.RuTiO_(2)/MXene@CC could achieve a high current density of 1000 mA·cm^(−2)at a small overpotential of 220 mV,superior to commercial dimensionally stable anodes(DSA).This study provides a new strategy for constructing efficient CER catalysts at high current density.

关键词： chlorine evolution reaction high current density MXene TiO_(2) RuO_(2)

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Graphdiyne scaffold anchored highly dispersed ruthenium nanoparticles as an efficient cathode catalyst for rechargeable Li-CO_(2) battery

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Chinese Chemical Letters 2024年第1期35卷 552-557页

作者： Yiru Ma Huiqi Qu Wenna Wang Ziyang Guo Yueqin Yu Feng Liu Bin Yu Minge Tian Zhenjiang Li Bin Li Lei Wang College of Chemistry and Molecular Engineering State Key Laboratory Base of Eco-Chemical EngineeringInternational Science and Technology Cooperation Base of Eco-Chemical Engineering and Green ManufacturingQingdao University of Science and TechnologyQingdao 266042China College of Materials science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China Biomedical Sensing Engineering Technology research Center Shandong UniversityJi'nan 250100China Scientific Green(shandong)Environmental Technology Co. Ltd.Jining Economic Development ZoneJining 272499China

Lithium (Li)-CO_(2) battery is rising as an attractive energy-storage system with the competence of CO_(2) conversion/fixation. However, its practical development is seriously hindered by the high overpotential. Herein, a rational design on a highly catalytic Li-CO_(2) battery electrode built by graphdiyne powder as a multi-functional laminar scaffold with anchored highly dispersed Ru nanoparticles is explored. The strong interaction between the abundant acetylenic bond sites of graphdiyne scaffold and Ru nanoparticles can effectively promote the electrochemical progress and reduce the voltage polarization. The unique channels architecture of the cathodic catalyst with enough space not only accelerates CO_(2) diffusion and electrons/Li+ transport, but also allows a large amount of accommodation for discharged product (Li2CO3) to assure an advanced capacity. The corresponding Li-CO_(2) battery displays an advanced discharged capacity of 15,030 mAh/g at 500 mA/g, great capacity retention of 8873 mAh/g at 2 A/g, high coulombic efficiency of 97.6% at 500 mA/g and superior life span for 120 cycles with voltage gap of 1.67 V under a restricted capacity of 1000 mAh/g at 500 mA/g. Ex/in-situ studies prove that synergy between Ru nanoparticles and acetylene bonds of GDY can boost the round-trip CO_(2)RR and CO_(2)ER kinetics.

关键词： Nanopores Li-CO_(2)battery Anchored Ru nanoparticles Graphdiyne Synergistic effect

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