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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

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

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

Yolk-shell structure synergistic defect engineering for boosting electromagnetic wave absorption in Co_(9)S_(8)@Humins-derived carbon

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Journal of Materials Science & Technology 2023年第33期164卷 140-149页

作者： Na Liang Zixu Yin Jingyun Guo Wanying Fang Qi Wang Ge Tian Dong Zhang Huijuan Yue shouhua feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education) College of PhysicsJilin UniversityChangchun 130012China

Exploring new strategies to incorporate the concepts of green chemistry and defect engineering into new architectures to address the problem of severe electromagnetic wave(EMW)pollution is challenging.In this work,by using a by-product of catalytic conversion of biomass as a carbon source,we prepare two-dimensional(2D)Co_(9)S_(8)-coated humins-derived carbon nanomaterials with a yolk-shell structure.The EMW attenuation ability is finally optimized by controlling the morphology and defects of the composite material through the pyrolysis temperature.As expected,with the synergy of conductive loss/interfacial polarization and defects regulating,the composite material achieves a reflection loss(RL)value of−51.4 dB in Ku-band and the effective absorption bandwidth(EAB)can be as high as 5.92 GHz(12.08–18.00 GHz)at 1.8 mm ultra-thin coating thickness.A strong absorption capacity in the low-frequency C-band(6.4 GHz)reaches RL value of−49.9 dB and a thickness of 3.50 mm,which grants it the characteristic of convertible microwave absorption from high frequency to low frequency.Taking account of the facile synthesis and tunable absorption properties,the encouraging findings shed light on exploring waste-turned-microwave absorbents with promising practical applications.

关键词： Yolk-shell structure Electromagnetic wave absorption Sulfide Humins

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

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

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

Electron transfer in Cu/Cu_(2)O generated by disproportionation promoting efficient CO_(2)photoreduction

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Nano Research 2022年第8期15卷 7099-7106页

作者： Qian Zhu Kainan Zhu Minmin Cai Yaowen Zhang Zhiyu Shao Mengpei Jiang Xiyang Wang Zhibin Geng Xiaofeng Wu Manrong Li Keke Huang shouhua feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin Provincial International Cooperation Key Laboratory of Advanced Inorganic Solid Functional Materials College of ChemistryJilin UniversityChangchun 130012China Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Constructing a high-efficiency composite material for CO_(2)photoreduction is a key step to the achievement of carbon neutralization,but a comprehensive understanding of the factors that dictate CO_(2)reduction activity remains elusive.Here,we constructed a series of Cu in situ combined on Cu_(2)O(Cu/Cu_(2)O-1,-2,-3)via an acid disproportionation method with various processing time.The optimal photocatalyst(Cu/Cu_(2)O-2)affords CO at a rate of 10.43μmol·g^(−1)·h^(−1),which is more than fourfold to that of pristine Cu_(2)O.Electron transfer in the samples was detected by X-ray absorption spectroscopy(XAS)as well as X-ray photoelectron spectroscopy(XPS).Interestingly,the best photoreduction performance was not achieved by the sample possessing the most electron transfer(Cu/Cu_(2)O-1)but by the one with moderate electron transfer(Cu/Cu_(2)O-2).By virtue of density functional theory(DFT)calculations,a linear relationship between Bader charge variation(Δq)of the active sites and adsorption energy of CO_(2)reduction intermediates was discovered,wherein the moderate charge transfer corresponds to appropriate adsorption energy,which benefits CO_(2)photoreduction activity substantially.This work provides guidance for the construction of composite catalysts for efficient CO_(2)photoreduction in a perspective of the quantity of electron transfer.

关键词： CO_(2)photocatalytic conversion charge transfer composite density functional theory(DFT)

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