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Highly Defective Dark TiO_(2) Modified with Pt: Effects of Precursor Nature and Preparation Method on Photocatalytic Properties

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Transactions of Tianjin University 2024年第2期30卷 198-209页

作者： E.D.Fakhrutdinova O.A.Reutova T.A.Bugrova I.Yu.Ovsyuk L.S.Kibis O.A.Stonkus D.B.Vasilchenko O.V.Vodyankina V.A.Svetlychnyi National Research Tomsk State University TomskRussia 634050 Novosibirsk State University NovosibirskRussia 630090 Boreskov institute of Catalysis NovosibirskRussia 630090 nikolaev institute of inorganic chemistry NovosibirskRussia 630090

The study focused on the modification with platinum of dark defective titania obtained via pulsed laser ablation. Both the method of Pt introduction and the nature of the Pt precursor were varied. All samples exhibited similar phase compositions, specific surface areas, and Pt contents. High-resolution transmission electron microscopy coupled with pulsed CO adsorption revealed increased dispersity when photoreduction and the hydroxonitrate complex (Me _(4) N) _(2) [Pt _(2) (OH) _(2) (NO _(3) ) _(8) ] were used. The sample featured a high content of single-atom species and subnano-sized Pt clusters. The X-ray photoelectron spectroscopy results showed that the photoreduction method facilitated the appearance of a larger number of Pt ^(2+) states, which appeared owing to the strong metal-support interaction (SMSI) eff ect of the transfer of electron density from the electron-saturated defects on the TiO _(2) surface to Pt ^(4+) . In the hydrogen evolution reaction, samples with a significant fraction of the Pt ^(2+) ionic component, capable of generating short-lived Pt^(0) single-atom sites under irradiation due to the SMSI eff ect, exhibited the highest photocatalytic activity. The 0.5Pt(C)/TiO_(2) -Ph sample exhibited the highest hydrogen yield with a quantum efficiency of 0.53, retaining its activity even after 8 h of operation.

关键词： Dark(black)TiO_(2) Pulsed laser ablation Platinum reduction method Precursor type Photocatalysis Hydrogen evolution reaction

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Electrostatic Interaction-directed Construction of Hierarchical Nanostructured Carbon Composite with Dual Electrical Conductive Networks for Zinc-ion Hybrid Capacitors with Ultrastability

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Energy & Environmental Materials 2024年第1期7卷 184-192页

作者： Changyu Leng Zongbin Zhao Xuzhen Wang Yuliya V.Fedoseeva Lyubov G.Bulusheva Alexander V.Okotrub Jian Xiao Jieshan Qiu State Key Lab of Fine Chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical Engineering Dalian University of TechnologyDalian 116024China nikolaev institute of inorganic chemistry Siberian Branch of the Russian Academy of Sciences3 Acad.Lavrentiev Ave.Novosibirsk 630090Russia College of Chemical Engineering Beijing University of Chemical Technology Beijing 100029China

Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy ***,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid ***,we report a bidirectional electrostatic generated self-assembly strategy to achieve the precisely controlled coatings of single-layer nanoscale MOFs on a range of substrates,including carbon nanotubes(CNTs),graphene oxide(GO),MXene,layered double hydroxides(LDHs),MOFs,and SiO_(2).The obtained MOF-based nanostructured carbon composite exhibits the hierarchical porosity(V_(meso)/V_(micro)∶2.4),ultrahigh N content of 12.4 at.%and"dual electrical conductive networks."The assembled aqueous zinc-ion hybrid capacitor(ZIC)with the prepared nanocarbon composite as a cathode shows a high specific capacitance of 236 F g^(-1)at 0.5 A g^(-1),great rate performance of 98 F g^(-1)at 100 A g^(-1),and especially,an ultralong cycling stability up to 230000 cycles with the capacitance retention of 90.1%.This work develops a repeatable and general method for the controlled construction of MOF coatings on various functional substrates and further fabricates carbon composites for ZICs with ultrastability.

关键词： carbon composite electrostatic interaction metal-organic framework coating self-assembly zinc-ion hybrid capacitor

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Surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

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Hydrochar and synthetic natural gas co-production for a full circular economy implementation via hydrothermal carbonization and methanation:An economic approach

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Journal of Environmental Sciences 2024年第6期140卷 69-78页

作者： Judith González-Arias Guillermo Torres-Sempere Miriam González-Castaño Francisco MBaena-Moreno Tomás RReina inorganic chemistry Department and Materials Sciences institute University of Seville-CSICSevilleSpain Materials Sciences institute(ICMSE) CSIC-University of SevilleSevilleSpain Department of chemistry and Chemical Engineering Chalmers University of TechnologyGothenburgSE 41296Sweden

Herein we study the economic performance of hydrochar and synthetic natural gas coproduction from olive tree *** process entails a combination of hydrothermal carbonization and *** a previous work,we evidenced that standalone hydrochar production via HTC results ***,we propose a step forward on the process design by implementing a methanation,adding value to the gas effluent in an attempt to boost the overall process techno-economic *** different plant capacities were analyzed(312.5,625 and 1250 kg/hr).The baseline scenarios showed that,under the current circumstances,our circular economy strategy in *** analysis of the revenues shows that hydrochar selling price have a high impact on NPV and subsidies for renewable coal production could help to boost the profitability of the *** the contrary,the analysis for natural gas prices reveals that prices 8 times higher than the current ones in Spain must be achieved to reach *** seems unlikely even under the presence of a strong subsidy *** costs analysis suggests that a remarkable electricity cost reduction or electricity consumption of the HTC stage could be a potential strategy to reach profitability ***,significant reduction of green hydrogen production costs is deemed instrumental to improve the economic performance of the *** results show the formidable techno-economic challenge that our society faces in the path towards circular economy societies.

关键词： Hydrothermal carbonization CO_(2)waste valorization Methanation Profitability analysis

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CO oxidation under lean and stoichiometric conditions over ceriazirconia with very low metal contents(Cu,Co,Ag and Pt)

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Journal of Rare Earths 2024年第9期42卷 1669-1681,I0002页

作者： J.C.Martínez-Munuera M.P.Yeste A.García-García MCMA Group Department of Inorganic Chemistry and Institute of MaterialsUniversity of AlicanteCarretera de San Vicente del Raspeig s/n03690San Vicente del RaspeigAlicanteSpain Solid chemistry and Catalysis Group Department of Materials ScienceMetallurgic Engineering and Inorganic ChemistryInstitute of Electronic Microscopy and Materials ResearchUniversity of CádizAp.40E-11510Puerto RealCádizSpain

In this work,several ceria-zirconia based catalysts with very lo w(and equimolar) metal contents were prepared,characterised and tested for the CO oxidatio n reaction(under lean and stoichiometric conditions),trying to emulate those conditions found in a diesel oxidation catalyst(DOC) system from a diesel engine and those encountered under gasoline exhaust(λ=1).The metals chosen are Cu,Co,Ag and Pt(as a reliable benchmark).The results reveal enormous differences among reducibility and catalytic activity despite quite similar structural and textural properties of the catalysts,showing differences among dispersion(Ag-catalyst seems to present a low level of dispersion).This catalyst seems to be characterised,as well,by a strong electronic interaction between Ce and Ag centres which is suggested to yield an improved reducibility under H_(2)-TPR ***,the order in catalytic activity(Cu>Ag>Co≈Pt>>support) seems not to follow the order found in reducibility and the Cu-catalyst seems to be the most active independently on the reaction conditions,yielding nearly overlapped CO oxidation catalytic *** restingly,a stro ng correlation between the catalytic activity under the two conditions tested and the OSC values of the Ce_(0.8)Zr_(0.2)O_(2)-supported metal catalysts is ***,OSC parameter measured at 150℃ can be used as a relevant descriptor to evaluate the CO oxidation activity at low and medium conversions for the investigated catalysts,much better than the H_(2)-TPR measurements.

关键词： CO oxidation Low metal content Ceria-zirconia Copper species OSC parameter Rare earths

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Nickel-based cerium zirconate inorganic complex structures for CO_(2)valorisation via dry reforming of methane

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Journal of Environmental Sciences 2024年第6期140卷 12-23页

作者： Juan Luis Martín-Espejo Loukia-Pantzechroula Merkouri Jesús Gándara-Loe José Antonio Odriozola Tomas Ramirez Reina Laura Pastor-Pérez Department of inorganic chemistry and Material Sciences institute of Seville University of Seville-CSICSeville 41092Spain Department of Chemical and Process Engineering University of SurreyGuildford GU27XHUnited Kingdom

The increasing anthropogenic emissions of greenhouse gases(GHG)is encouraging extensive research in CO_(2)*** reforming of methane(DRM)depicts a viable strategy to convert both CO_(2)and CH4into syngas,a worthwhile chemical *** the different active phases for DRM,the use of nickel as catalyst is economically favourable,but typically deactivates due to sintering and carbon *** stabilisation of Ni at different loadings in cerium zirconate inorganic complex structures is investigated in this work as strategy to develop robust Ni-based DRM *** and TPR-H2analyses confirmed the existence of different phases according to the Ni loading in these ***,superficial Ni is observed as well as the existence of a CeNiO_(3)perovskite *** catalytic activity was tested,proving that 10 wt.%Ni loading is the optimum which maximises *** catalyst was also tested in long-term stability experiments at 600and 800℃in order to study the potential deactivation issues at two different *** 600℃,carbon formation is the main cause of catalytic deactivation,whereas a robust stability is shown at 800℃,observing no sintering of the active phase evidencing the success of this strategy rendering a new family of economically appealing CO_(2)and biogas mixtures upgrading catalysts.

关键词： CO_(2)conversion Dry reforming of methane Nickel catalysts Pyrochlore Cerium zirconate

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Synergistic Co-doping effect of CNTs and PVP in Na_(4)MnCr(PO_(4))3 cathode as a strategy for improving the electrochemical performance of SIBs

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Chinese Chemical Letters 2024年第2期35卷 539-543页

作者： Ruoyu Chen Denys S.Butenko Shilin Li Xinyu Zhang Guangshe Li Igor V.Zatovsky Wei Han College of Physics State Key Laboratory of Inorganic Synthesis and Preparative ChemistryInternational Center of Future ScienceJilin UniversityChangchun 130012China Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhen 518055China State Key Laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China F.D.Ovcharenko institute of Biocolloidal chemistry NAS UkraineKyiv 03142Ukraine

In order to solve the contradiction between the rapidly growing energy demand and the excessive exploitation of fossil fuels,it is urgent to research and develops more environmentally friendly and efficient energy storage ***,the development of high-performance cathode materials to enhance the energy density of SIB is currently one of the most important topics of scientific *** high-voltage and low-cost cathode material for SIBs,a composite of carbon-coated Na_(4)MnCr(PO_(4))_(3)(NASICON-type),polyvinylpyrrolidone(PVP),and modified carbon nanotubes(CNTs)is prepared by sol-gel and freeze-drying *** to the high conductivity of CNTs,the conductivity of the composite is significantly improved,and its initial capacity is increased to 114 mAh/g at 0.5 C and 96 mAh/g at 5 C(Mn^(2+)/Mn^(4+)conversion for voltage windows 1.4-4.3 V).Moreover,the multi-electrons transfer of Cr^(3+)/Cr^(4+) and Mn^(2+)/Mn^(4+) can provide a high capacity of 165 mAh/g at 0.1 C and 102 mAh/g at 5 C in the high voltage window of 1.4-4.6 ***,PVP can effectively inhibit the Jahn-Teller effect caused by Mn ion,making the composite have more excellent high-rate performance and *** addition,GITT,EIS and CV curves were drawn to better reveal the excellent kinetic properties of Na_(4)MnCr(PO_(4))_(3)@C@PVP@CNT cathode,and the mechanism of its performance improvement is deeply studied and ***,the co-doping of CNTs and PVP is a simple way to high conductivity and fast charging of cathode materials for SIBs.

关键词： Sodium-ion batteries Na_(4)MnCr(PO_(4))_(3) Carbon nanotubes Polyvinylpyrrolidone Synergistic effect

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Nanozyme catalysis in a crowded environment:The impact of diffusion and surface shielding

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Nano Research 2024年第7期17卷 5795-5800页

作者： Vasily G.Panferov Juewen Liu Department of chemistry Waterloo Institute for NanotechnologyWaterlooOntario N2L 3G1Canada

Nanozymes are widely used in various applications as nanosized catalysts for replacing *** accurate estimation of the catalytic activity of nanozymes in real conditions is *** this article,for the first time,we systematically studied the effect of macromolecular molecules co-existing in the real system on the oxidoreductase(peroxidase,oxidase,and catalase)-mimicking nanozymes made of a gold nanoparticle core and a platinum shell,Prussian Blue,Mn_(2)O_(3) and CoO *** were made with horseradish *** distinguished two main mechanisms of the negative impact of macromolecules on nanozyme catalysis—slowed diffusion and surface shielding of *** the first mechanism is typical for enzymes,the second one is specific only for *** the mechanisms is essential for developing approaches to reduce the unavoidable impact of macromolecules for various analytical and biomedical applications.

关键词： molecular crowding biosensors nanoparticles

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Low-temperature replacement construction of three-dimensional corrosion-resistant interface for deeply rechargeable Zn metal batteries

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Nano Materials Science 2024年第3期6卷 329-336页

作者： Jinze Li Daniel Rohrens Gianluca Dalfollo Xiaochao Wu Ziheng Lu Qiang Gao Bo Han Ruimin Sun Chenggang Zhou Jindi Wang Zhao Cai Faculty of Materials Science and chemistry China University of GeosciencesWuhan430074China institute of inorganic chemistry RWTH Aachen UniversityAachen52074Germany Microsoft Research AI4Science Beijing10080China institute of New Energy on Chemical Storage and Power Sources College of Applied Chemistry and Environmental EngineeringYancheng Teachers UniversityYancheng224000China

Aqueous Zn batteries are promising candidates for grid-scale renewable energy *** electrodes have been widely investigated and applied as anode materials for aqueous Zn batteries,however,they suffer from limited surface area and severe interfacial issues including metallic dendrites and corrosion side reactions,limiting the depth of discharge(DOD)of the foil electrode ***,a low-temperature replacement reaction is utilized to in-situ construct a three-dimensional(3D)corrosion-resistant interface for deeply rechargeable Zn foil ***,the deliberate low-temperature environment controlled the replacement rate between polycrystalline Zn metal and oxalic acid,producing a Zn foil electrode with distinct 3D corrosion-resistant interface(3DCI-Zn),which differed from conventional two-dimensional(2D)protective structure and showed an order of magnitude higher surface ***,the 3DCI-Zn electrode exhibited dendrite-free and anticorrosion properties,and achieved stable plating/stripping performance for 1000 h at 10 mA cm^(-2)and 10 mAh cm^(-2)with a remarkable DOD of 79%.After pairing with a MnO2cathode with a high areal capacity of 4.2 mAh cm^(-2),the pouch cells delivered 168 Wh L^(-1)and a capacity retention of 89.7%after 100 cycles with a low negative/positive(N/P)ratio of 3:1.

关键词： Aqueous batteries Foil electrodes Depth of discharge Dendrites Corrosion side reactions

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Boosting oxygen reduction activity and CO_(2) resistance on bismuth ferrite-based perovskite cathode for low-temperature solid oxide fuel cells below 600℃

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Journal of Energy chemistry 2024年第3期90卷 600-609,I0013页

作者： Juntao Gao Zhiyun Wei Mengke Yuan Zhe Wang Zhe Lü Qiang Li Lingling Xu Bo Wei School of Physics Harbin Institute of TechnologyHarbin 150001HeilongjiangChina Key Laboratory of Functional inorganic Material chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080HeilongjiangChina School of Physics and Electronic Engineering Harbin Normal UniversityHarbin 150025HeilongjiangChina

Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical ***,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for *** doping can significantly enhance the electrocata lytic activity and chemical stability of *** 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious *** remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi ***,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) *** work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.

关键词： Low-temperature solid oxide fuel cell Perovskite cathode DFT calculations CO_(2) tolerance

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