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Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO_(2. photoreduction via alternately hydrophobic surfaces

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Journal of Energy chemistry 2024年第6期93卷 202-212,I0006页

作者： Hailing Huo Ting Hu chengxi Huang fang Wu Tongyu Wang Xuan Liu Liang Zhang Qiang Ju Zhiqing Zhong Hongbin {2. Erjun Kan Ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina college of Information Science and Technology Nanjing Forestry UniversityNanjing 210037JiangsuChina

The overall photocatalytic CO_(2. reduction reaction(OPCRR)that can directly convert CO_(2. and H_(2.O into fuels represents a promising renewable energy conversion *** a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2. reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of ***,there is a contradiction in wettability requirements for the two ***,CRHR prefers a hydrophobic surface that can accumulate more CO_(2. molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2.)to liquid-phase(H_(2.O)***,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2.)from the catalyst surface,preventing isolation between active sites and the reactant(H_(2.O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic *** was achieved through a selectively hydrophobic modification method and a charge-transfer-control ***,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(2.1.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark *** innovative approach holds great potential for application in universal overall reactions involving gas participation.

关键词： Hydrophobic Hydrophilic Gas transport Overall CO_(2.photoreduction Z-scheme

Study of the Voltammetric Behavior of Heme and Its Direct Analysis Application

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wuhan university Journal of Natural {2. 1998年第4期3卷 473-475页

作者： Liu Huihong Ye Baoxian zhou xing{2.(college of chemistry, wuhan university, wuhan 430072, china) wuhan university College of Chemistry Wuhan China (GRID:grid.49470.3e) (ISNI:***)

The electroanalytical method of ferriheme was studied by linear sweep voltammetry in medium of 0.05 mol/L Tris+0.05 mol/L NH3?NH4Cl buffer at hang mercury drop electrodes (HMDE). Heme exhibits two pair reversible redox peaks and one irreversible peak. The cathodic peak potentials are?;0.2.6 V, ?0.42. V and ?1.408 V respectively. The first and the third peaks can be used for directly quantitative determination of heme concentrations. The peak currents are good linear relationship with heme concentration in ranges of 3×10?6–6×10?5 mol/L and 3×10?7–1.5×10?5 mol/L respectively.

关键词： heme voltammetric behavior catalytic wave

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 Yuan{2. 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 2..0μmol/hr(i.e.,2.00μmol/(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)

An aqueous magnesium-ion hybrid supercapacitor operated at-50℃

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Green Energy & Environment 2024年第4期9卷 702-712页

作者： Guoshen Yang Gangrui Qu Chi fang Jie Deng Xianqi Xu Yinghao Xie Tian Sun Yachao Zhu Jiaxin Zheng Hang zhou School of Electronic and Computer Engineering Peking University Shenzhen Graduate SchoolShenzhen518055China School of Advanced Materials Peking University Shenzhen Graduate SchoolShenzhenChina college of Food and Biological Engineering Chengdu UniversityChengdu610106China Institute Charles Gerhardt Montpellier UMR 5253Universitae MontpellierMontpellierCC 1502France

The recent advances in aqueous magnesium-ion hybrid supercapacitor(MHSC)have attracted great attention as it brings together the benefits of high energy density,high power density,and synchronously addresses cost and safety ***,the freeze of aqueous electrolytes discourages aqueous MHSC from operating at low-temperature ***,a low-concentration aqueous solution of 4 mol L^(-1) Mg(ClO_(4))_(2. is devised for its low freezing point(-67℃)and ultra-high ionic conductivity(3.37 mS cm^(-1) at-50℃).Both physical characterizations and computational simulations revealed that the Mg(ClO_(4))_(2. can effectively disrupt the original hydrogen bond network among water molecules via transmuting the electrolyte structure,thus yielding a low freezing ***,the Mg(ClO_(4))_(2. electrolytes endue aqueous MHSC with a wider temperature operation range(-50℃–2.℃)and a higher energy density of 103.9 Wh kg^(-1) at 3.68 kW kg^(-1) over commonly used magnesium salts(i.e.,MgSO_(4) and Mg(NO_(3))_(2.)***,a quasi-solid-state MHSC based on polyacrylamide-based hydrogel electrolyte holds superior low-temperature performance,excellentﬂexibility,and high *** work pioneers a convenient,cheap,and eco-friendly tactic to procure low-temperature aqueous magnesium-ion energy storage device.

关键词： Low-concentration aqueous electrolyte Anti-freezing property Magnesium-ion hybrid supercapacitor High energy density

NiO@Ni nanoparticles embedded in N-doped carbon for efficient photothermal CO_(2. methanation coupled with H_(2.O splitting

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Nano Research 2024年第4期17卷 2283-2290页

作者： Yun zhou Peng Zheng fang Wang fangna Gu Wenqing Xu Qinyang Lu Tingyu Zhu Ziyi Zhong Guangwen Xu Fabing Su Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China Key Laboratory on Resources Chemicals and Materials of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China Institute of Industrial chemistry and Energy Technology Shenyang University of Chemical TechnologyShenyang 110142China School of Ecology and Environment Beijing Technology and Business UniversityBeijing 100048China Beijing Key Laboratory of Enze Biomass Fine Chemicals College of New Materials and Chemical EngineeringBeijing Institute of Petrochemical TechnologyBeijing 102617China International School of Beijing 10 An Hua Street Shunyi DistrictBeijing 100048China Department of Chemical Engineering Guangdong Technion Israel Institute of Technology(GTIIT)Shantou 515063China Technion Israel Institute of Technology(IIT) Haifa32000Israel

Photothermal carbon dioxide(CO_(2.)methanation has attracted increasing interest in solar fuel synthesis,which employs the advantages of photocatalytic H_(2.O splitting as a hydrogen source and photothermal catalytic CO_(2. *** work prepared three-dimensional(3D)honeycomb N-doped carbon(NC)loaded with core–shell NiO@Ni nanoparticles generated in situ at 500℃(NiO@Ni/NC-500).Under the photothermal catalysis(2.0℃,1.5 W/cm^(2.),the CH_(4) evolution rate of NiO@Ni/NC-500 reached 5.5 mmol/(g·h),which is much higher than that of the photocatalysis(0.8 mmol/(g·h))and the thermal catalysis(3.7 mmol/(g·h)).It is found that the generated localized surface plasmon resonance enhances the injection of hot electrons from Ni to NiO,while thermal heating accelerates the thermal motion of radicals,thus generating a strong photo-thermal synergistic effect on the *** CO_(2. reduction to CH_(4) follows the*OCH *** work demonstrates the synergistic effect of NiO@Ni and NC can enhance the catalytic performance of photothermal CO_(2. reduction reaction coupled with water splitting reaction.

关键词： Ni localized surface plasmon resonance photothermal methanation

An Efficient Multifunctional Soluble Catalyst for Li-O_(2. Batteries

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CCS chemistry 2024年第7期6卷 1810-1820页

作者： Shuochao xing Zhengcai Zhang Yaying Dou Minghui Li Jing Wu Zhang Zhang Zhen zhou Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2. School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001 Key Laboratory of Advanced Energy Materials chemistry Ministry of EducationCollege of ChemistryNankai UniversityTianjin 300071

Aprotic lithium-oxygen(Li-O_(2.)batteries have a high theoretical energy density,but they face challenges such as cathode blockage,high charge overpotential,and poor cycling *** are caused by sluggish reaction kinetics and severe parasitic *** the performance of Li-O_(2. batteries necessitates the development of efficient *** catalysts not only augment both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)but also inhibit undesirable parasitic *** this work,we demonstrated for the first time a multifunctional soluble catalyst of iridium(III)acetylacetonate(Ir(acac)_(3))that could speed up oxygen ***(acac)_(3) regulated the ORR pathway and the reactivity of superoxide radical species by forming a reversible intermediate complex(Ir(acac)_(3)-O_(2.^(−)).During charging,Ir(acac)_(3) acted as a redox mediator and aided in Li_(2.O_(2. decomposition by reacting with superoxide ***,as demonstrated by operando UV-visible spectroscopy,the lower charge potential significantly reduced the generation of highly reactive singlet oxygen(^(1)O_(2.)*** a result,the Ir(acac)_(3)-mediated Li-O_(2. battery showed low overpotential,large capacity,and stable *** study offers a new approach to achieving efficient Li-O_(2. batteries and provides an opportunity to suppress parasitic reactions.

关键词： Li-O_(2.battery soluble catalyst superoxide species organometallics singlet oxygen

Three-Component Transformation of CO_(2.,Propargyl Alcohols and Secondary Amines intoβ-Oxopropylcarbamates Promoted by a Noble Metal-Free Metal–Organic Framework Catalyst

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CCS chemistry 2024年第9期6卷 2333-2345页

作者： Xiao-Lei Jiang fang-Yu Ren Ying Shi yao Xie Sheng-Li Hou Bin Zhao Department of chemistry Key Laboratory of Advanced Energy Material Chemistry(Ministry of Education)MOERenewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300071 college of chemistry and Chemical Engineering Yantai UniversityYantai 264010

The three-component reaction of CO_(2.,propargyl alcohols,and secondary amines frequently applies noble metal or homogeneous catalysts,therefore it is necessary and important to seek a recyclable catalyst without noble metals for this reaction,despite the multitude of ***,a unique framework{[Ce3(Cu4I4)2.CNA)8(DMF)8](NO3)}n(CuCe-CNA)with two kinds of metal cluster nodes[Ce3]and[Cu4I4]was synthesized,displaying high thermal and chemical ***-CNA-300 was obtained by removing the coordinated DMF molecules with[Ce3]cluster at 300°C,in which more metal sites are exposed and the pores are enlarged,but the three-dimensional framework still remains ***-CNA-300 can effectively catalyze the three-component reaction of 2.methyl-3-butyn-2.alcohol,CO_(2.,and pyrrolidine toβ-oxopropylcarbamates with a yield of 98%under mild conditions,and the catalytic activity is higher than those of noble metal ***,CuCe-CNA-300 exhibits high catalytic efficiency for various kinds of propargyl alcohols and secondary amines,and also shows good *** studies suggest that theα-alkylidene cyclic carbonates derived from the cycloaddition of propargyl alcohols and CO_(2. are the intermediates,which further react with secondary amines through ammonolysis reaction to generateβ-***,this work may open a new avenue for the one-pot transformation of CO_(2. with two or more components into value-added chemicals activated by noble metal-free metal–organic frameworks catalysts.

关键词： three-component reaction CO_(2.conversion metal-organic frameworks noble metal-free catalyst synergistic catalysis

The Crystallization Behavior of L-Poly(lactic acid)/Polypropylene Blends:The Acceleration for Both L-Poly(lactic acid)and Polypropylene

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Chinese Journal of Polymer Science 2024年第6期42卷 775-786页

作者： Shuang-cheng Li Wei-Jia zhou Wen-Jie Wu Jun Shao Shui-Liang Chen Hao-Qing Hou Sheng Xiang college of chemistry&Chemical Engineering and Nanofiber Engineering Center of Jiangxi Province Jiangxi Normal UniversityNanchang330022China National Engineering Research Center for Carbohydrate Synthesis/Key Lab of Fluorine and Silicon for Energy Materials and chemistry of Ministry of Education Jiangxi Normal UniversityNanchang330022China Wenzhou Institute University of Chinese Academy of SciencesWenzhou325001China

For a polymer/polymer dismissible blend with two crystallizable components,the crystallization behavior of different components and the reciprocal influences between different crystals are interesting and important,but did not investigate in *** this study,the L-poly(lactic acid)/polypropylene(PLLA/PP)blends with different weight ratios were prepared by melt mixing and the crystallization behavior of the blends were *** showed that the crystalline structures of PLLA and PP were not altered by the *** the crystallization of PLLA,both the diffusion of chain segments and crystallization rate were enhanced under the existence of PP *** the crystallization of PP,its crystallization rate was depressed under the existence of amorphous PLLA molecular *** the PP crystallized from the existence of PLLA crystals,although the diffusion rate of PP was reduced by PLLA crystals,the nucleation positions were obviously enhanced,which accelerated the formation of PP *** investigation would supply more basic data for the application of PLLA/PP blend.

关键词： L-poly(lactic acid) Polypropylene Blends Crystalization behavior Crystallization acceleration

Statistical theory for hydrogen bonding fluid system of A_aD_d type (I): The geometrical phase transition

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Science china chemistry 2006年第6期49卷 499-506页

作者： WANG Haijun1,2. HONG Xiaozhong3, GU fang1 & BA Xinwu1 1. college of {2. and Environment Science, Hebei university, Baoding 071002. china 2. International Center for Materials Physics, Chinese Academy of sciences, Shenyang 110016, china 3. college of Physics Science and Technology, Hebei university, Baoding 071002. china 1. college of chemistry and Environment Science Hebei University Baoding 071002 China 2. International Center for Materials Physics Chinese Academy of Sciences Shenyang 110016 China 3. college of Physics Science and Technology Hebei University Baoding 071002 China

The influence of hydrogen bonds on the physical and chemical properties of hydrogen bonding fluid system of AaDd type is investigated from two viewpoints by the principle of statistical mechanics. In detail, we proposed two new ways that can be used to obtain the equilibrium size distribution of the hydrogen bonding clusters, and derived the analytical expression of a relationship between the hydrogen bonding free energy and hydrogen bonding degree. For the nonlinear hydrogen bonding systems, it is shown that the sol-gel phase transition can take place under proper conditions, which is further proven to be a kind of geometrical phase transition rather than a thermodynamic one. Moreover, several problems associated with the geometrical phase transition and liquid-solid phase transition in nonlinear hydrogen bonding systems are discussed.

关键词： hydrogen bonding fluid, equilibrium free energy, geometrical phase transition.