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Carbon energy 2024年第1期6卷 255-266页

作者： Qianying Lin Jiwu Zhao Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin Ding Rusheng Yuan Xuxu Wang Jinlin Long State Key Laboratory of Photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhouChina

Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great ***,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic *** exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and ***,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) *** study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.

关键词： artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC

S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO_(3)nanoparticles for photocatalytic CO_(2)reduction

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Journal of environmental Sciences 2024年第6期140卷 103-112页

作者： Gongjie Chen Ziruo Zhou Bifang Li Xiahui Lin Can Yang Yuanxing Fang Wei Lin Yidong Hou Guigang Zhang Sibo Wang State Key Laboratory of Photocatalysis on energy and environment College of ChemistryFuzhou UniversityFujian 350116China

Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting;however,their mission in light-driven CO_(2)conversion remains to be *** this work,crystalline carbon nitride(CCN)nanosheets of poly triazine imide(PTI)embedded with melon domains are fabricated by KCl/LiCl-mediated polycondensation of dicyandiamide,the surface of which is subsequently deposited with ultrafine WO_(3)nanoparticles to construct the CCN/WO_(3)heterostructure with a S-scheme *** characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO_(3)hybrid,featuring strengthened optical capture,enhanced CO_(2)adsorption and activation,attractive textural properties,as well as spatial separation and directed movement of light-triggered charge *** mild conditions,the CCN/WO_(3)catalyst with optimized composition displays a high photocatalytic activity for reducing CO_(2)to CO in a rate of 23.0μmol/hr(i.e.,2300μmol/(hr·g)),which is about 7-fold that of pristine CCN,along with a high CO selectivity of 90.6%against ***,it also manifests high stability and fine reusability for the CO_(2)conversion *** CO_(2)adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS),identifying the crucial intermediates of CO_(2)^(*)-,COOH^(*)and CO^(*),which integrated with the results of performance evaluation proposes the possible CO_(2)reduction mechanism.

关键词： Crystalline carbon nitride Photocatalysis CO_(2)reduction S-scheme WO_(3)

Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao Institute of Catalysis for energy and environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high *** study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) *** further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and ***,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate *** H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/*** calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational ***,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) *** indicted that the chemisorptions of aldehyde oxygen have largest *** results suggested adsorption conformations have a respectable impact on the catalysis *** study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO_(4)catalyst

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Chinese Chemical Letters 2024年第3期35卷 171-176页

作者： Fen Wei Weichao Xue Zhiyang Yu Xue Feng Lu Sibo Wang Wei Lin Xinchen Wang State Key Laboratory of Photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350108China

Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant ***,we present that an oxygen vacancy(O_v)-rich LaVO_(4)(LaVO_(4)-O_v)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(O_(latt.))and O_(v)co-mediated *** by simulated sunlight at mild conditions,LaVO_(4)-O_(v)effectively dehydrogenates undiluted ethane to produce C_(2)H_(4)and CO with a conversion of 2.3%.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C_(2)H_(4)are enhanced to 275μmol h^(-1)g^(-1)and 96.8%.Of note,LaVO_(4)-O_(v)appears nearly no carbon deposition after the *** isotope tracked reactions reveal that the consumed O_(latt.)recuperates by exposing the used catalyst with O_(2),thus establishing a dynamic cycle of O_(latt.)and achieving a facile catalyst regeneration to preserve its intrinsic *** refreshed LaVO_(4)-O_(v)exhibits superior reusability and delivers a turnover number of about *** O_(v)promotes photo absorption,boosts ethane adsorption/activation,and accelerates charge separation/transfer,thus improving the photocatalytic *** possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).

关键词： Photocatalysis Ethane dehydrogenation Ethene LaVO_(4) Oxygen vacancy

Rational design of practical layered transition metal oxide cathode materials for sodium-ion batteries

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Frontiers of Chemical Science and Engineering 2024年第7期18卷 121-140页

作者： Yan Wang Ning Ding Rui Zhang Guanhua Jin Dan Sun Yougen Tang Haiyan Wang Hunan Provincial Key Laboratory of Chemical Power sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China college of energy and Chemical Engineering Xinjiang Institute of TechnologyAksu Prefecture 843100China

Sodium-ion batteries (SIBs), which serve as alternatives or supplements to lithium-ion batteries, have been developed rapidly in recent years. Designing advanced high-performance layered NaxTMO_(2) cathode materials is beneficial for accelerating the commercialization of SIBs. Herein, the recent research progress on scalable synthesis methods, challenges on the path to commercialization and practical material design strategies for layered NaxTMO_(2) cathode materials is summarized. Co-precipitation method and solid-phase method are commonly used to synthesize NaxTMO_(2) on mass production and show their own advantages and disadvantages in terms of manufacturing cost, operative difficulty, sample quality and so on. To overcome drawbacks of layered NaxTMO_(2) cathode materials and meet the requirements for practical application, a detailed and deep understanding of development trends of layered NaxTMO_(2) cathode materials is also provided, including high specific energy materials, high-entropy oxides, single crystal materials, wide operation temperature materials and high air stability materials. This work can provide useful guidance in developing practical layered NaxTMO_(2) cathode materials for commercial SIBs.

关键词： sodium-ion batteries layered oxide industrialization development prospect

Metal-free two-dimensional phosphorene-based electrocatalyst with covalent P-N heterointerfacial reconstruction for electrolyte-lean lithium-sulfur batteries

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Carbon energy 2024年第5期6卷 175-185页

作者： Jiangqi Zhou Chengyong Shu Jiawu Cui Chengxin Peng Yong Liu Weibo Hua Laura Simonelli Yuping Wu Shi Xue Dou Wei Tang School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina School of Materials Science and Engineering University of Shanghai for Science and TechnologyShanghaiChina State Key Laboratory of Space Power-sources Technology Shanghai Institute of Space Power-SourcesShanghaiChina CELLS-ALBA Synchrotron BarcelonaSpain School of energy and environment Southeast UniversityNanjingChina

The use of lithium-sulfur batteries under high sulfur loading and low electrolyte concentrations is severely restricted by the detrimental shuttling behavior of polysulfides and the sluggish kinetics in redox ***-dimensional(2D)few layered black phosphorus with fully exposed atoms and high sulfur affinity can be potential lithium-sulfur battery electrocatalysts,which,however,have limitations of restricted catalytic activity and poor electrochemical/chemical *** resolve these issues,we developed a multifunctional metal-free catalyst by covalently bonding few layered black phosphorus nanosheets with nitrogen-doped carbon-coated multiwalled carbon nanotubes(denoted c-FBP-NC).The experimental characterizations and theoretical calculations show that the formed polarized P-N covalent bonds in c-FBP-NC can efficiently regulate electron transfer from NC to FBP and significantly promote the capture and catalysis of lithium polysulfides,thus alleviating the shuttle ***,the robust 1D-2D interwoven structure with large surface area and high porosity allows strong physical confinement and fast mass ***,with c-FBP-NC as the sulfur host,the battery shows a high areal capacity of 7.69 mAh cm^(−2) under high sulfur loading of 8.74 mg cm^(−2) and a low electrolyte/sulfur ratio of 5.7μL mg^(−1).Moreover,the assembled pouch cell with sulfur loading of 4 mg cm^(−2) and an electrolyte/sulfur ratio of 3.5μL mg^(−1) shows good rate capability and outstanding *** work proposes an interfacial and electronic structure engineering strategy for fast and durable sulfur electrochemistry,demonstrating great potential in lithium-sulfur batteries.

关键词： black phosphorus electronic structure high sulfur loading interfacial covalent bonds lean electrolyte

Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction

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Molecular dynamics study of water molecules nucleation for fine particle removal:Effects of wettability and aggregation modes and comparison with experiment Author links open overlay panel

结构化学 2024年第3期43卷 10-18页

作者： Ziruo Zhou Wenyu Guo Tingyu Yang Dandan Zheng Yuanxing Fang Xiahui Lin Yidong Hou Guigang Zhang Sibo Wang State Key Laboratory of Photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou350116China college of environment and Safety Engineering Fuzhou UniversityFuzhou350108China

Sunlight-induced photocatalytic carbon dioxide(CO2)reduction to energy-rich chemicals by metal-free polymeric carbon nitride(CN)semiconductor is a promising tactic for sustained solar fuel ***,the reaction efficiency of CO2 photoreduction is restrained seriously by the rapid recombination of photogenerated carriers on CN ***,we incorporate 2-aminopyridine molecule with strong electron-withdrawing group into the skeleton edge of CN layers through a facile one-pot thermal polymerization strategy using urea as the precursor,which renders a modified carbon nitride(ACN)with extended optical harvesting,abundant nitrogen defects and ultrathin nanosheet ***,the ACN photocatalyst with desirable structural features attains enhanced separation and migration of photoexcited charge *** visible light irradiation with Co(bpy)32+as a cocatalyst,the optimized ACN sample manifests a high CO2 deoxygnative reduction activity and high sta-bility,providing a CO yielding rate of 17 μmol h-1,which is significantly higher than that of pristine *** key intermediates engaged in CO2 photoreduction reaction are determined by the in situ diffuse reflectance infrared Fourier transform spectroscopy,which sponsors the construction of the possible photocatalytic CO2 reduction mechanism on ACN nanosheets.

关键词： Carbon nitride Photocatalysis CO_2 reduction Nitrogen defects Nanosheets

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Particuology 2024年第8期91卷 106-117页

作者： Junchao Xu Zhipeng Zhang Li Lv Yunfei Zhang Yiming Xie Huaqiang Chu School of energy and environment Anhui University of TechnologyMaanshan243002China college of Mechanical and Electrical Engineering China Jiliang UniversityHangzhou310018China

Water vapor nucleation on particle's surface plays an important role in dust removal,cloud formation,and particle ***,the selectivity of nucleation sites and the nucleation characteristic of water molecule on the particle's surface are still unclear,especially for the aggregated *** this paper,the effects of particle wettability and aggregation modes on the selectivity of nucleation sites and the nucleation characteristics were investigated using molecular dynamics *** results were compared with our earlier experimental *** illustrates how the contact angle of clusters,the growth velocity,and the growth duration are all influenced by the interaction coefficient between water and ***,the nucleation sites of water molecules on the particle aggregation surface exhibit a definite *** primary indicator of this selectivity is the preferential nucleation of water molecules at the interfaces of linear chain aggregation particles,at the inner side of non-linear chain aggregation particles,and at the centers of ring *** results are in good agreement with our previous experimental *** significantly,additional research has revealed that subcritical-size clusters typically aggregate on two-particle surfaces spacing when the spacing smaller than the critical cluster size.

关键词： Heterogeneous nucleation Water molecule Wettability Aggregation modes Molecule dynamics

Harnessing data using symbolic regression methods for discovering novel paradigms in physics

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Science China(Physics,Mechanics & Astronomy) 2024年第6期67卷 1-11页

作者： Jianyang Guo Wan-Jian Yin college of energy Soochow Institute for Energy and Materials Innovations(SIEMIS)Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy TechnologiesSoochow UniversitySuzhou 215006China Shanghai Qi Zhi Institute Shanghai 200232China Light Industry Institute of Electrochemical Power sources Soochow UniversitySuzhou 215006China

In recent years,machine-learning methods have profoundly impacted research in the interdisciplinary fields of ***,most machine-learning models lack interpretability,and physicists doubt the credibility of their conclusions because they cannot be combined with prior physical ***,this review focuses on symbolic regression,which is an interpretable machine-learning ***,the relevant concepts of machine learning are introduced in conjunction with ***,we provide an overview of symbolic regression ***,the recent directions for the application of symbolic regression methods in different subfields of physics are outlined,and an overview of the ways in which the applications of symbolic regression have evolved in the realm of physics is *** major aim of this review is to introduce the basic principles of symbolic regression and explain its applications in the field of physics.

关键词： machine learning genetic programming symbolic regression

Extended light absorption and accelerated charge migration in ultrathin twisted carbon nitride nanoplates for efficient solar hydrogen production

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Science China Chemistry 2024年第7期67卷 2215-2223页

作者： Yanmin Zou Shiyao Li Dandan Zheng Jianyong Feng Sibo Wang Yidong Hou Guigang Zhang State Key Laboratory of Photocatalysis on energy and environment College of ChemistryFuzhou UniversityFuzhou 350108China college of environment and Safety Engineering Fuzhou UniversityFuzhou 350108China Collaborative Innovation Center of Advanced Microstructures National Laboratory of Solid State MicrostructuresCollege of Engineering and Applied SciencesNanjing UniversityNanjing 210093China

Polymeric carbon nitride has been widely developed as a promising photocatalyst for solar hydrogen production via photocatalytic water ***,pristine carbon nitride prepared by traditional solid-state polymerization usually encounters issues such as rapid carrier recombination and insufficient absorption of visible light below 460 ***,poly(heptazine imide)with a distinctive nanoplate structure was synthesized in a binary molten salt of NaCl–CaCl_(2).The salt template allows the formation of the thin nanoplate structure,which promotes the charge separation and ***,the intercalation of Ca^(2+)ions between the conjugated layers endows the activation of n–π*electron transition due to the distortion of in-plane heptazine ***,the optimized poly(heptazine imide)nanoplates achieve an apparent quantum efficiency of up to 17.3%at 500 nm for photocatalytic hydrogen production from *** work shares new idea for rational control of the optical absorption and charge carrier dynamics of poly(heptazine imide).

关键词： photocatalysis poly heptazine imide nanoplates ion intercalation hydrogen production