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Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang key laboratory of catalysis and energy materials chemistry of ministry of education&hubei key laboratory of catalysis and materials science South-Central Minzu UniversityWuhan 430074China hubei key laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique structures.The structural sensitivity of these catalysts is closely linked to their particle size and crystal form.Consequently,comprehending the structure–activity relationship requires the development of well-defined Co-based catalysts.Herein,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon nanospheres.The nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO nanoparticles.By adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal forms.The influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been investigated.The result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 nm.However,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(<7.7 nm).Significantly,when metallic fcc-Co^(0) particle size was reduced from 17.6 to 7.7 nm,the cobalt time yield increased to 6.7μmolCO·gCo^(-1)·s^(-1),indicating improved catalytic activity.At the same time,the CH_(4) selectivity decreased to 4.9%,suggesting a higher preference for hydrocarbon production.These findings demonstrate the importance of particle size in Co catalyzed Fischer–Tropsch synthesis.The use of well-defined CoO/CS catalysts offers valuable insights into the structure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

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Copper-catalyzed C(sp)-H aryl amination enables modular synthesis of quinolines and 2-quinolinones

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science China chemistry 2024年第2期67卷 595-603页

作者： Yang Gao Haixia Li Simin Yang Yanping Huo Qian Chen Xianwei Li Zhe Wang Xiao-Qiang Hu School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou510006China Jieyang Branch of chemistry and Chemical Engineering Guangdong laboratory Jieyang515200China key laboratory of catalysis and energy materials chemistry of ministry of education&hubei key laboratory of catalysis and materials science School of Chemistry and Materials ScienceSouth-Central University for NationalitiesWuhan430074China

Herein,we disclose a novel copper-catalyzed C(sp)-H aryl amination of terminal alkynes with anthranils,enabling the rapid generation of highly reactive secondary N-aryl ynamines for the modular synthesis of structurally diverse C2-substituted quinolines and 2-quinolinones.The in-situ formed carbonyl-ynamines are prone to tautomerize to carbonyl-ketenimines,which can efficiently react with a series of nucleophiles,including amines,alcohols,phenols,thiols,thiophenols,active-methylene compounds,and even water to produce various quinoline derivatives with the generation of H_(2)O as a sole and green byproduct.This method also unlocks a practical route to create various quinoline-fused heterocycles and can be successfully applied to the late-stage modification of complex molecules and the concise synthesis of bioactive targets.Mechanistic studies reveal a coppercatalyzed inner-sphere nitrene transfer process by using anthranils as novel aryl nitrene precursors.

关键词： copper catalysis anthranils C(sp)-H aryl amination carbonyl-ketenimines quinolines

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Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient oxidative self-coupling of benzylamines

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Frontiers of Chemical science and Engineering 2024年第1期18卷 95-106页

作者： Jie Chen Mingyuan Jian Deqiong Xie Kecan Dou Deli Chen Weidong Zhu Fumin Zhang key laboratory of the ministry of education for Advanced catalysis materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

In this study,we synthesize a catalyst comprising cobalt nanoparticles supported on MXene by pyrolyzing a composite in a N2 environment.Specifically,the composite comprises a bimetallic Zn/Co zeolitic imidazole framework grown in situ on the outer surface of MXene.The catalytic efficiency of the catalyst is tested for the self-coupling of 4-methoxybenzylamine to produce value-added imine,where atmospheric oxygen(1 atm)is used as the oxidant.Based on the results,the catalyst displayed impressive catalytic activity,achieving 95.4%yield of the desired imine at 383 K for 8 h.Furthermore,the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional groups.The outstanding performance of the catalyst is primarily attributed to the synergetic catalytic effect between the cobalt nanoparticles and MXene support,while also benefiting from the three-dimensional porous structure.Additionally,a preliminary investigation of potential reaction mechanisms is conducted.

关键词： MXene sacrificial template oxidative self-coupling Co nanoparticles imine

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Recent progress in photocatalytic NAD(P)H regeneration for photocatalytic-enzymatic-coupling system

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Frontiers of Chemical science and Engineering 2024年第4期18卷 1-24页

作者： Wei Lan Maodi Wang Huicong Dai Qihua Yang key laboratory of the ministry of education for Advanced catalysis materials Zhejiang Key Laboratory for Reactive Chemistry on Solid SurfacesInstitute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

The enzymatic redox reactions in natural photosynthesis rely much on the participation of cofactors,with reduced nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate(NADH/NADPH)or their oxidized form(NAD+/NADP+)as an important redox power.The photocatalytic regeneration of expensive and unstable NADH/NADPH in vitro is an important process in enzymatic reduction and has attracted much research attention.Though different types of photocatalysts have been developed for photocatalytic NADH/NADPH regeneration,the efficiency is still relatively low.To elucidate the key factors affecting the performance of photocatalytic NADH/NADPH regeneration is helpful to rationally design the photocatalyst and improve the photocatalytic efficiency.In this paper,we overview the recent progress in photocatalytic NADH/NADPH regeneration with the focus on the strategies to improve the visible light adsorption,the charge separation and migration efficiency,as well as the surface reaction,which jointly determine the overall photocatalytic regeneration efficiency.The potential development of photocatalytic NADH/NADPH regeneration and photocatalyticenzymatic-coupling system is prospected finally.

关键词： photocatalytic-enzymatic coupling NAD(P)H regeneration photocatalysis efficiency

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Ultrafast micro/nano-manufacturing of metastable materials for energy

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National science Review 2024年第4期11卷 283-298页

作者： Xiaoya Cui Yanchang Liu Yanan Chen School of materials science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education) and Tianjin Key Laboratory of Composite and Functional MaterialsTianjin University ministry of education key laboratory of Protein sciences School of Life SciencesTsinghua University

The structural engineering of metastable nanomaterials with abundant defects has attracted much attention in energy-related fields. The high-temperature shock(HTS) technique, as a rapidly developing and advanced synthesis strategy, offers significant potential for the rational design and fabrication of high-quality nanocatalysts in an ultrafast, scalable, controllable and eco-friendly way. In this review, we provide an overview of various metastable micro-and nanomaterials synthesized via HTS, including single metallic and bimetallic nanostructures, high entropy alloys, metal compounds(e.g. metal oxides) and carbon nanomaterials. Note that HTS provides a new research dimension for nanostructures, i.e. kinetic modulation. Furthermore, we summarize the application of HTS—as supporting films for transmission electron microscopy grids—in the structural engineering of 2D materials, which is vital for the direct imaging of metastable materials. Finally, we discuss the potential future applications of high-throughput and liquid-phase HTS strategies for non-equilibrium micro/nano-manufacturing beyond energy-related fields.It is believed that this emerging research field will bring new opportunities to the development of nanoscience and nanotechnology in both fundamental and practical aspects.

关键词： high-temperature shock technique defect engineering metastable phase kinetic modulation non-equilibrium micro/nano-manufacturing

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Dilute Aqueous-Aprotic Electrolyte Towards Robust Zn-Ion Hybrid Supercapacitor with High Operation Voltage and Long Lifespan

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Nano-Micro Letters 2024年第9期16卷 1-12页

作者： Shuilin Wu Yibing Yang Mingzi Sun Tian Zhang Shaozhuan Huang Daohong Zhang Bolong Huang Pengfei Wang Wenjun Zhang key laboratory of catalysis and energy materials chemistry of ministry of education&hubei key laboratory of catalysis and materials science South-Central Minzu UniversityWuhan 430074People’s Republic of China Department of materials science and Engineering and Center of Super‑Diamond and Advanced FilmsCity University of Hong Kong83 Tat Chee AvenueKowloon TongHong Kong SARPeople’s Republic of China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China key laboratory of Photochemical Conversion and Optoelectronic materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijingPeople’s Republic of China

With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required.However,the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan.It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.Using'water in salt'electrolytes can effectively broaden their electrochemical windows,but this is at the expense of high cost,low ionic conductivity,and narrow temperature compatibility,compromising the electrochemical performance of the Zn-ion hybrid supercapacitors.Thus,designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary.We developed a dilute water/acetonitrile electrolyte(0.5 m Zn(CF_(3)SO_(3))_(2)+1 m LiTFSI-H_(2)O/AN)for Zn-ion hybrid supercapacitors,which simultaneously exhibited expanded electrochemical window,decent ionic conductivity,and broad temperature compatibility.In this electrolyte,the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI-anions.As a result,a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.

关键词： Zn-ion supercapacitors Zn metal anode Electrolyte engineering Hydrogen bonds Solvation structures

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Pd Pt VO_(x)/CeO_(2)-ZrO_(2):Highly efficient catalysts with good sulfur dioxide-poisoning reversibility for the oxidative removal of ethylbenzene

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Journal of Environmental sciences 2024年第4期138卷 153-166页

作者： Jia Wang Yuxi Liu Jiguang Deng Lin Jing Xiuqing Hao Xing Zhang Xiaohui Yu Hongxing Dai Beijing key laboratory for Green catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.

关键词： Ceria-zirconia Supported palladium-platinum-vanadium catalyst Volatile organic compound Ethylbenzene oxidation Sulfur dioxide resistance

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Enhanced photocatalytic nitrogen fixation performance via in situ constructing BiO_(2-x)/NaNbO_(3) heterojunction

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Chinese Journal of Chemical Engineering 2024年第5期69卷 92-100页

作者： Jiayu Zhang Zhihao Zeng Lin Yue Chunran Zhao Xin Hu Leihong Zhao Xiuwen Wang Yiming He key laboratory of the ministry of education for Advanced catalysis materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China Heilongjiang Provincial key laboratory of Surface Active Agent and Auxiliary School of Chemistry and Chemistry EngineeringQiqihar UniversityQiqihar 161006China Department of materials science and Engineering Zhejiang Normal UniversityJinhua 321004China

The fabrication of heterojunction catalysts is an effective strategy to enhance charge separation efficiency,thereby boosting the performance of photocatalysts.In this study,BiO_(2-x)nanosheets were synthesized through a hydrothermal process and loaded onto NaNbO_(3) microcube to construct a series of BiO_(2-x)/NaNbO_(3) heterojunctions for photocatalytic N_(2) fixation.Results indicated that 2.5%BiO_(2-x)/NaNbO_(3) had the highest photocatalytic performance.The NH_(3) production rate under simulated solar light reached 406.4μmol·L^(-1)·g^(-1)·h^(-1),which reaches 2.6 and 3.8 times that of NaNbO_(3) and BiO_(2-x),respectively.BiO_(2-x)nanosheets primarily act as electron trappers to enhance the separation efficiency of charge carriers.The strong interaction between BiO_(2-x)and NaNbO_(3) facilitates the electron migration between them.Meanwhile,the abundant oxygen vacancies in BiO_(2-x)nanosheets may facilitate the adsorption and activation of N_(2),which may be another possible reason of the high photocatalytic activity of the BiO_(2-x)/NaNbO_(3).This study may offer new insights for the development of semiconductor materials in photocatalytic nitrogen fixation.

关键词： Catalyst Solar energy Hydrothermal BiO_(2-x)/NaNbO_(3) Photocatalytic N_(2)-fixation

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Revisiting the sodium-ion storage capability of hard carbon in carbonate-based electrolytes via a sodium-metal-free protocol

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science China chemistry 2024年第7期67卷 2240-2247页

作者： Gaopan Liu Yanbing Mo Jiawei Chen Yu Peng Xiao Zhu Fei Wang Xiaoli Dong Yongyao Xia Department of chemistry and Shanghai key laboratory of Molecular catalysis and Innovative materials Institute of New EnergyLaboratory of Advanced MaterialsFudan UniversityShanghai 200438China

Common evaluation methodology of sodium(Na)-containing two-electrode or three-electrode configurations overlooks the interference from highly reactive Na metal,leading to the underestimation or inconsistent performance of low-potential hard carbon(HC)electrodes.Herein,the trap of Na metal was systematically investigated with or without applied current,uncovering its inadequacy as the reference or counter electrode in different configurations.A Na-metal-free three-electrode protocol is proposed for evaluating the actual Na^(+)-storage capability of the typical low-potential HC electrode.By avoiding Na crosstalk and precisely controlling the working electrode's potential,the actual electrochemical performance of HC in the carbonate esterbased electrolyte can be recognized with high capacity of 222 mAh g^(-1)at 2 C and 113 mAh g^(-1)at 5 C,correcting the misunderstanding of the inferior performance of HC in coin-type half cells(68%and 50%undervaluation at 2 C and 5 C,respectively).The advanced protocol is expected to reduce misunderstandings or underestimation due to evaluation methods and to guide the development of high-performance battery materials.

关键词： highly reactive sodium potential drift carbonate ester sodium-metal-free protocol sodium storage capability

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Synergism of solar-driven interfacial evaporation and photo-Fenton Cr(VI)reduction by sustainable Bi-MOF-based evaporator from waste polyester

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Journal of energy chemistry 2024年第7期94卷 527-540页

作者： Zifen Fan Jie Liu Huajian Liu Lijie Liu Yan She Xueying Wen Huiyue Wang Guixin Hu Ran Niu Jiang Gong key laboratory of Material chemistry for energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringHuazhong University of Science andTechnologyWuhan430074HubeiChina

The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(VI)-polluted water remains challenging,and the synergistic mechanism on Cr(VI)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MoF microrod from waste poly(ethylene terephthalate),and construct Bi-MoF-based solar evaporators for simultaneous photo-Fenton Cr(VI)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MoF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(VI)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(VI)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(vI)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(VI).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.

关键词： Interfacial solar steam generation Cr(VI)reduction Photo-Fenton reaction Metal-organic framework Waste plastic upcycling

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