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Optimizing the electronic spin state and delocalized electron of NiCo_(2)(OH)_(x)/MXene composite by interface engineering and plasma boosting oxygen evolution reaction

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Journal of Energy Chemistry 2022年第8期31卷 129-140,I0004页

作者： Jingyao Xu Xia Zhong Xiaofeng Wu Ying Wang Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012JilinChina Chinese Acad Sci Inst Met ResShenyang Natl Lab Mat SciShenyang 110016LiaoningChina Univ Sci&Technol China Sch Mat Sci&EngnShenyang 110016LiaoningChina State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

The electrocatalytic activity of transition-metal-based compounds is closely related to the electronic configuration.However,optimizing the surface electron spin state of catalysts remains a challenge.Here,we developed a spin-state and delocalized electron regulation method to optimize oxygen evolution reaction(OER)performance by in-situ growth of NiCo_(2)(OH)_(x) using Oswald ripening and coordinating etching process on MXene and plasma treatment.X-ray absorption spectroscopy,magnetic tests and electron paramagnetic resonance reveal that the coupling of NiCo_(2)(OH)_(x) and MXene can induce remarkable spin-state transition of Co^(3+)and transition metal ions electron delocalization,plasma treatment further optimizes the 3 d orbital structure and delocalized electron density.The unique Jahn-Teller phenomenon can be brought by the intermediate spin state(t2 _(g)^(5) e_(g)^(1))of Co^(3+),which benefits from the partial electron occupied egorbitals.This distinct electron configuration(t2_(g)^(5) e_(g)^(1))with unpaired electrons leads to orbital degeneracy,that the adsorption free energy of intermediate species and conductivity were further optimized.The optimized electrocatalyst exhibits excellent OER activity with an overpotential of 268 m V at 10 m A cm^(-2).DFT calculations show that plasma treatment can effectively regulate the d-band center of TMs to optimize the adsorption and improve the OER activity.This approach could guide the rational design and discovery of electrocatalysts with ideal electron configurations in the future.

关键词： Transition metal compounds Electronic state control of surface/interface Electron spin state Delocalized electron Electrocatalytic material

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Strong High Entropy Alloy-Support Interaction Enables Efficient Electrocatalytic Water Splitting at High Current Density

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Chinese Journal of Structural Chemistry 2022年第8期41卷 3-11页

作者： Hongdong Li Yue Pan Jianping Lai Lei Wang Shouhua Feng Key Laboratory of Eco-chemical Engineering Taishan Scholar Advantage and Characteristic Discipline Team of Eco-chemical Process and TechnologyCollege 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

In electrocatalysis, the stability issue between catalyst and support still needs great attention. Here, a series of highentropy alloy nanoparticles(HEA-NPs) embedded in carbon cloth(CC) were synthesized by using the scalable strategy-microwave heating. Among them, PtRhCoNiCu/CC exhibits outstanding hydrogen evolution reaction(HER) activity(19 and 170 mV overpotential at 10 and 1000 mA cm^(-2)) and stability(150 h), outperforming other recently reported HEAs catalysts. IrRuCoNiCu/CC displays superior oxygen evolution reaction(OER) activity(166 and 354 mV overpotential at 10 and 1000 m A cm^(-2)) and stability(150 h), and shows a lower overpotential than recently reported HEA catalysts. In water splitting, IrRuCoNiCu/CC(+)//Pt Rh Co Ni Cu/CC(-) electrolyzer achieves 500 m A cm^(-2)(1000 m A cm^(-2)) high current density at 1.76 V(1.88 V) and exhibits excellent stability, which is one of the best catalysts currently. Therefore, the novel supported HEA catalyst with high stability is expected to be a promising candidate material for industrialized water splitting.

关键词： high entropy alloy metal-support interactions microwave heating water splitting activity and durability

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New perspective on the synthesis of highly efficient composites:regulating influence distance of interfacial charge transfer

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Science Bulletin 2018年第4期63卷 203-205页

作者： Keke Huang Zhibin Geng Yu Sun Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University

Interface effect is one of the central topics for decades[1–3].For inorganic composites,interface effect is mainly induced by interface stress[4]and interface charge transfer[4–6],in which interface charge transfer ... 详细信息

关键词：费用距离界面调整合成电子状态化学性质接口

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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 barriers.Therefore,achieving high CH_(4) activity and selectivity remains a significant challenge.Here,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*CHO.The 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 reaction.This 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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Coordination engineering of cobalt phthalocyanine by functionalized carbon nanotube for efficient and highly stable carbon dioxide reduction at high current density

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Nano Research 2022年第4期15卷 3056-3064页

作者： Hongdong Li Yue Pan Zuochao Wang Yaodong Yu Juan Xiong Haoyang Du Jianping Lai Lei Wang Shouhua Feng Key Laboratory of Eco-chemical Engineering Taishan scholar advantage and characteristic discipline team of Eco-chemical process and technologyCollege 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

Coordination engineering can enhance the activity and stability of the catalyst in heterogeneous catalysis.However,the axial coordination engineering between different groups on the carbon carrier and molecular catalysts in the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR)has been studied rarely.Through coordination engineering strategy,a series of amino(NH_(2)),hydroxyl(OH),and carboxyl(COOH)groups functionalized carbon nanotubes(CNT)immobilized cobalt phthalocyanine(CoPc)catalysts are designed.Compared with no groups,OH groups and COOH groups,NH_(2)groups can effectively change the coordination environment of the central metal Co,thereby significantly increasing the turnover frequency(TOF)(31.4 s^(-1)at-0.6 V vs.RHE,CoPc/NH_(2)-CNT>CoPc/OH-CNT>CoPc/COOH-CN>CoPc/CNT).In the flow cell,the CoPc/NH_(2)-CNT catalyst has high carbon monoxide(CO)selectivity at high current density(~100%at-225 mA·cm^(-2),~96%at-351 mA·cm^(-2)).Importantly,the CoPc/NH_(2)-CNT catalyst can operate stably for 100 h at 225 mA·cm^(-2).Theoretical calculations reveal that CoPc/NH_(2)-CNT catalyst is beneficial to the formation of^(*)COOH and desorption of^(*)CO,thus promoting CO_(2)RR.This work provides an excellent platform for understanding the effect of coordination engineering on electrocatalytic performance and promotes a way to explore efficient and stable catalysts in other applications.

关键词： cobalt phthalocyanine(CoPc) functionalized carbon nanotubes(CNT) coordination engineering highly stable carbon dioxide electroreduction

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Rational design of interfacial bonds within dual carbon-protected manganese oxide towards durable aqueous zinc ion battery

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Science China Chemistry 2023年第5期66卷 1406-1416页

作者： Xiuli Guo Chunguang Li Xiyang Wang Zhenhua Li Hui Zeng Pan Hou Minggang Xie Yuxin Li Zhan Shi Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Department of Mechanical and Mechatronics Engineering Waterloo Institute for NanotechnologyMaterials Interface FoundryUniversity of WaterlooWaterlooOntario N2L 3G1Canada

Manganese-based cathode materials are promising candidates for aqueous zinc ion batteries(AZIBs)by reason of their low cost and high energy density.However,their practical applicability is hampered by the intrinsic defects of poor electrical conductivity,sluggish reaction kinetics,and severe structural deterioration.Herein,we constructed a hierarchically porous structure composed of carbon-encapsulated Mn O nanoparticles(MOC)and three-dimensional(3D)nitrogen-doped graphene aerogel(NGA)(denoted as MOC@NGA).The hybrid was synthesized by a facile in-situ coprecipitation and annealing of manganesebased metal-organic framework(Mn-MOF74)and NGA composite(Mn-MOF74@NGA).Specifically,the carbon shells inherited from organic ligand of Mn-MOF74 could restrain the volume changes of Mn O,and the porous NGA prevented the agglomeration of MOC nanoparticles and enriched the types of interfacial chemical bonds.Profiting from the synergistic effect of rich interface chemical bonds and dual-carbon protection,the MOC@NGA hybrids exhibit fast interfacial electron/charge transfer and transport,and outstanding structural stability.Therefore,MOC@NGA cathode delivers an excellent rate performance(270 and 99.8 m Ah g^(-1)at 0.1 and 2.0 A g^(-1))and maintains an excellent specific capacity of 151.6 m Ah g^(-1)after 2,000cycles at 1.0 A g^(-1).Moreover,the fabricated MOC@NGA-based quasi-solid-state battery not only achieves outstanding flexibility but also displays impressive cycling stability,demonstrating a promising potential for portable and flexible equipment.This work provides a feasible strategy for the fabrication of the bridging structure of manganese-based oxides and porous carbon matrix for high-specific capacity and durable AZIBs cathodes.

关键词： manganese oxide interfacial chemical bonds carbon modification aqueous zinc ion batteries

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Enhanced CO catalytic oxidation by Sr reconstruction on the surface of LaxSr1-xCoO3-δ

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Science Bulletin 2017年第9期62卷 658-664页

作者： Xiyang Wang Keke Huang Jingyu Qian Yingge Cong Chengda Ge Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry filin University Changchun 130012 China State Key Laboratory of Supramolecular Structure and Materials College of Chemistry filin University Changchun 130012 China

Surface electronic structure of solid materials plays a critical role in heterogeneous catalysis. However,surface chemical composition of the perovskite oxides is usually dominated by segregated A-site cations and the amount of oxygen vacancies is relatively low, which seriously restricts their catalytic oxidation property. Here, we prepare perovskite La_xSr_(1-x)CoO_(3-δ)(x = 0.3, 0.5, 0.7) with different Sr doping amount and experiment results show that perovskite LSCO with higher content of surface Sr possesses more oxygen vacancies and better catalytic activity. On this basis, we develop a new experimental strategy to create more surface oxygen vacancies to promote their CO catalytic activity. In this method, we use high active hydrogen atoms(BH^(4-)) as reductant to realize surface in-situ chemical composite modification of La_xSr_(1-x)CoO_(3-δ)(x = 0.3, 0.5, 0.7), which causes their surface reconstruction(surface Sr enrichment).The regulation mainly focuses on the atomic layer level without damaging their bulk phase structure.Different from traditional high temperature annealing under reducing atmosphere, this method is high-efficiency, green and controllable. Furthermore, we study the surface reconstruction process and demonstrated that it is atomic layer engineering on the surface of La_xSr_(1-x)CoO_(3-δ)(x = 0.3, 0.5, 0.7) by X-ray photoelectron spectroscopy(XPS) and X-ray absorption fine structure(XAFS). Our experiment results also show that these samples treated by this method exhibit superior activity for CO oxidation compared with original samples.

关键词： Surface reconstruction KBH4 Perovskite oxides Oxygen vacancies CO oxidation

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Defect-engineered Mn_(3)O_(4)/CNTs composites enhancing reaction kinetics for zinc-ions storage performance

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Journal of Energy Chemistry 2022年第5期31卷 538-547页

作者： Xiuli Guo Hao Sun Chunguang Li Siqi Zhang Zhenhua Li Xiangyan Hou Xiaobo Chen Jingyao Liu Zhan Shi Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012JilinChina Laboratory of Theoretical and Computational Chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130023JilinChina School of Engineering RMIT UniversityCarltonVIC 3053Australia

The designing of reasonable nanocomposite materials and proper introduction of defect engineering are of great significance for the improvement of the poor electronic conductivity and slow reaction kinetics of manganese-based compounds. Herein, we report manganese-deficient Mn_(3)O_(4) nanoparticles which grow in-situ on highly conductive carbon nanotubes(CNTs)(denoted as DMOC) as an advanced cathode material for aqueous rechargeable zinc-ion batteries(RAZIBs). According to experimental and calculation results, the DMOC cathode integrates the advantages of enriched Mn defects and small particle size. These features not only enhance electronic conductivity but also create more active site and contribute to fast reaction kinetics. Moreover, the structure of DMOC is maintained during the charging and discharging process, thus benefiting for excellent cycle stability. As a result, the DMOC electrode delivers a high specific capacity of 420.6 m A h g^(-1) at 0.1 A g^(-1) and an excellent cycle life of 2800 cycles at 2.0 A g^(-1) with a high-capacity retention of 84.1%. In addition, the soft-packaged battery assembled with DMOC cathode exhibits long cycle life and high energy density of 146.3 Wh kg^(-1) at 1.0 A g^(-1) . The results are beneficial for the development of Zn/Mn_(3)O_(4) battery for practical energy storage.

关键词： Manganese oxide Manganese defects High rate Long cycle life Zinc ion batteries

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A Self-Strengthening Epidermis-Like Smart Coating Enabled by Dynamic Iron Sequestration

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CCS Chemistry 2021年第11期3卷 2655-2668页

作者： Xiaodong Qi Lei Yang Ying Hou Jiaqi Zhu Ming Yang Shouhua Feng Key Laboratory of Microsystems and Micronanostructures Manufacturing Harbin Institute of TechnologyHarbin 150080 State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun 130012

Living organisms rely on materials sequestration from the environment to strengthen their bodies.Such constant activity provides necessary supplies for critical biological functions,which is difficult by man-made structures due to the lack of a dynamic sequestration mechanism.In this study,it is shown that an epidermis-like smart coating can respond to changes in salinity to allow a spontaneous and progressive strengthening when supported by steel as a sustained iron source.The self-strengthening is enabled by reaction-coupled diffusion,which makes possible the dynamic sequestration of iron from the in situ rusted steel,partially mimicking the iron accumulation process in a mussel.The emergence of iron-phenolic coordination bonds continuously improves modulus,hardness,and adhesion,achieving a strengthening efficiency comparable to mussel byssus.Interestingly,the bilayer design ensures long-term self-healing performance even during strengthening and a mechanically robust anticorrosion coating with an autonomic protection mechanism and gradually enhanced barrier properties during prolonged service.Our results provide a new venue for the design of stimuli-responsive smart materials characteristic of an open biological system and may serve as the basis for creating highly intelligent devices with sophisticated functionality.

关键词： biomimetics self-strengthening selfhealing smart coating epidermis-like

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Dimensional reduction enhances photocatalytic carbon dioxide reduction performance of metal-organic frameworks

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Nano Research 2024年第5期17卷 3653-3659页

作者： Kaiyue Ma Jixin Li Jinlu Liu Chunguang Li Zhan Shi Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)have shown significant potential as photocatalysts.It has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be explored.In this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the literature.Re(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,respectively.Photocatalytic CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of 3D-MOF-Re.The result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb light.This study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.

关键词： photocatalysis CO_(2)reduction metal-organic frameworks(MOFs) nanosheets light absorption

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