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Combining anodic alcohol oxidative coupling for C-C bond formation with cathodic ammonia production

National Science Review 2024年第5期11卷 217-226页

作者： Leitao Xu Wei Chen Cairong Wang Wenjie Wu Yelin Yao Zhifeng Huang Jingcheng Wu Ming Yang Yandong Wu Dianke Xie Yuqin Zou Shuangyin Wang State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of Education Hunan University

Electrocatalytic oxidation of alcohols using heterogeneous catalysts is a promising aqueous, energy-efficient and environmentally friendly approach, especially for coupling different alcohols to prolong the carbon chain via co-oxidation. Precisely regulating critical steps to tailor electrode materials and electrolyte composition is key to selectively coupling alcohols for targeted synthesis. However, selectively coupling different alcohols remains challenging due to the lack of effective catalyst and electrolyte design promoting specific pathways. Herein, we demonstrate a paired electrolysis strategy for combining anodic oxidative coupling of ethanol（EtOH） and benzyl alcohol（PhCH2OH） to synthesize cinnamaldehyde（CAL） and cathodic ammonia production. The strategies involve:（i） utilizing the salt-out effect to balance selective oxidation and coupling rates;（ii） developing platinum-loaded nickel hydroxide electrocatalysts to accelerate intermediate coupling kinetics;（iii） introducing thermodynamically favorable nitrate reduction at the cathode to improve coupling selectivity by avoiding hydrogenation of products while generating valuable ammonia instead of hydrogen. We achieved 85% coupling selectivity and 278 μmol/h NH3productive rate at 100 m A/cm2with a low energy input（～1.63 V）. The membrane-free, low energy, scalable approach with a wide substrate scope highlights promising applications of this methodology. This work advances heterogeneous electrocatalytic synthesis through rational design principles that integrate anodic oxidative coupling with cathodic nitrate reduction reactions, having synergistic effects on efficiency and selectivity.

关键词： anodic alcohol oxidative coupling C–C bond formation cinnamaldehyde cathodic ammonia production

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Weak interaction-steered evolution of polyoxovanadate-based metal-organic polyhedra from transformation via interlock to packing

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Chinese chemical Letters 2024年第2期35卷 527-533页

作者： Yan-Hu Wang Ke-Wei Tong Chao-Qin Chen Jing Du Peng Yang college of chemistry and chemical engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China college of chemistry and Materials Science Testing and Analysis CenterHebei Normal UniversityShijiazhuang 050024China

A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak *** contrast with covalent bonds bearing definite orientation and high stability,weak intermolecular forces within a continuous dynamic equilibrium can be hardly tamed for molecular *** this endeavor,a ligand-dominated strategy that embodies tunable electrostatic repulsion andπ···πstacking was first employed to shape polyoxovanadate-based metal-organic polyhedra(VMOPs).Structural evolution involving transformation,interlock,and discovery of an unprecedented prototype of the Star of David was hence *** only as a handy tool for the primary structural control over VMOPs,these weak forces allow for an advanced management on the spatial distribution of such manmade macromolecules as well as the associated physicochemical behaviors,representing an ideal model for simulating and interpreting the conformation-function relationship of proteins.

关键词： Polyoxometalates Polyoxovanadates Metal-organic polyhedron Interlock Weak intermolecular forces

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Homogenous coating of Li^(+)conductive Li_(5)AlO_(4)on single-crystalline nonstoichiometric Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)for rechargeable lithium-ion batteries

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Journal of Energy chemistry 2024年第8期95卷 651-659,I0014页

作者： Guoyu Ding Shizhou Wang Jinhan Li Ziyan Wu Jiayu Chen Jiayong Du Xinhui Huang Kuiming Liu Yudong Zhang Zhonghan Wu Yiyang Peng Qiancheng Zhao Meng Yu Fangyi Cheng Key Laboratory of advanced Energy Materials chemistry(ministry of education) Engineering Research Center of High-efficiency Energy Storage(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of advanced chemical Power Sources Nankai UniversityTianjin 300071China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China

Cobalt-free,nickel-rich LiNi_(1-x)Al_(x)O_(2)(x≤0.1)is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate *** this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li_(5)AlO_(4)-coated single-crystalline slightly Li-rich Li_(1.04)Ni_(0.92)Al_(0.04)O_(2).The symbiotic formation of Li_(5)AlO_(4)from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li_(5)AlO_(4)that permits high Li^(+)*** from mitigated undesirable side reactions and phase evolution,the Li_(5)AlO_(4)-coated single-crystalline Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)delivers a high specific capacity of220.2 mA h g^(-1)at 0.1 C and considerable rate capability(182.5 mA h g^(-1)at 10 C).Besides,superior capacity retention of 90.8%is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full ***,the particulate morphology of Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li_(0.98)Ni_(0.97)Al_(0.05)O_(2)features intragranular cracks and irreversible lattice *** results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

关键词： Aluminum segregation Surface coating Nonstoichiometric oxides Molten synthesis Cathode materials

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Anodic Electrosynthesis of Amide from Alcohol and Ammonia

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CCS chemistry 2024年第1期6卷 125-136页

作者： Yuxuan Lu Yingying Li Bo Zhou Jingcheng Wu Ling Zhou Yuping Pan Zhongcheng Xia Ming Yang Yandong Wu Zhenran Yuan Rixin Peng Zhijie Kong Shuangyin Wang Yuqin Zou State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082 Shenzhen Institute of Hunan University Shenzhen 518057 School of chemistry and chemical engineering Jishou UniversityJishouHunan 416000

Amide is essential in biologically active compounds,synthetic materials,and building ***,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to construct the C–N ***,for the first time,we have successfully realized the formation of amides at industrial current density via the anodic coelectrolysis of alcohol and ammonia under ambient *** have proved thatmodulation of the interface microenvironment concentration of nucleophile by electrolyte engineering can regulate the reaction pathways of amides rather than acetic *** C-N coupling strategy can be further extended to the electrosynthesis of the long-chain and aryl-ring amide with high selectivity by replacing ammonia with *** work opens up a vast store of information on the utilization of biomass alcohol for high-value N-containing chemicals via an electrocatalytic C-N coupling reaction.

关键词： electrocatalysis electrocatalysts biomass upgrading elctrochemical oxidation coupling amide production

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Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Nano research 2024年第8期17卷 7163-7173页

作者： Huicong Xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan Key Laboratory of advanced Energy catalytic and Functional Material Preparation of Zhengzhou College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Key Laboratory of Materials Physics of ministry of education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China Key Laboratory of chemical Reaction engineering of Shaanxi Province College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China center for High Pressure Science and Technology advanced research PudongShanghai 201203China Key Laboratory of advanced Energy Materials chemistry(ministry of education) Nankai UniversityTianjin 300071China

In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount *** SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the ***,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been *** electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery *** functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during *** process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction ***,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关键词： Ti_(3)C_(2)/Fe-N-C heterostructure work-function electron interaction solid electrolyte interphase sodium storage

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Experimental and theoretical investigation of sulfur-doped g-C_(3)N_(4)nanosheets/FeCo_(2)O_(4)nanorods S-scheme heterojunction for photocatalytic H_(2)evolution

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Nano research 2024年第9期17卷 8007-8016页

作者： Haitao Wang Lianglang Yu Jiahe Peng Jing Zou Weiping Gong Jizhou Jiang School of chemistry and Environmental engineering School of Environmental Ecology and Biological EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Guangdong Provincial Key Laboratory for Electronic Functional Materials and Devices Huizhou UniversityHuizhou 516007China

g-C_(3)N_(4)emerges as a promising metal-free semiconductor photocatalyst due to its cost-effectiveness,facile synthesis,suitable visible light response,and robust thermal ***,its practical application in photocatalytic hydrogen evolution reaction(HER)is impeded by rapid carrier recombination and limited light absorption *** this study,we successfully develop a novel g-C_(3)N_(4)-based step-scheme(S-scheme)heterojunction comprising two-dimensional(2D)sulfur-doped g-C_(3)N_(4)nanosheets(SCN)and one-dimensional(1D)FeCo_(2)O_(4)nanorods(FeCo_(2)O_(4)),demonstrating enhanced photocatalytic HER *** engineered SCN/FeCo_(2)O_(4)S-scheme heterojunction features a well-defined 2D/1D heterogeneous interface facilitating directed interfacial electron transfer from FeCo_(2)O_(4)to SCN,driven by the lower Fermi level of SCN compared to FeCo_(2)O_(4).This establishment of electron-interacting 2D/1D S-scheme heterojunction not only facilitates the separation and migration of photogenerated carriers,but also enhances visible-light absorption and mitigates electron-hole pair *** structure analysis and density functional theory calculations corroborate that the carrier migration in the SCN/FeCo_(2)O_(4)photocatalyst adheres to a typical S-scheme heterojunction mechanism,effectively retaining highly reactive photogenerated ***,the optimized SCN/FeCo_(2)O_(4)heterojunction exhibits a substantially high hydrogen production rate of 6303.5μmol·g^(-1)·h^(-1)under visible light excitation,which is 2.4 times higher than that of the ***,the conjecture of the S-scheme mechanism is confirmed by in situ XPS *** 2D/1D S-scheme heterojunction established in this study provides valuable insights into the development of high-efficiency carbon-based catalysts for diverse energy conversion and storage applications.

关键词： g-C_(3)N_(4) FeCo_(2)O_(4) S-scheme heterojunction photocatalytic hydrogen evolution reaction(HER)

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Cobalt Single Atom-Catalyzed Formation of LiOH in Li-O_(2)Batteries via the Direct 4-Electron Oxygen Reduction Pathway

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CCS chemistry 2024年第10期6卷 2502-2514页

作者： Kang Huang Hao Wan Zhichao Gong Jianbin Liu Minmin Yan Jun Wu Chunyu Cui Gonglan Ye Karsten Reuter Huilong Fei advanced catalytic engineering research center of the ministry of education State Key Laboratory for Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082 Fritz-Haber-Institut der Max-Planck-Gesellschaft Berlin 14195

The formation of LiOH as the discharge product instead of Li_(2)O_(2)in Li-O_(2)batteries(LOBs)is highly desirable due to the associated drawbacks of Li_(2)O_(2)-based chemistry,which involves the generation of reactive oxygen intermediates responsible for substantial side ***,the current challenge lies in the formation pathway of LiOH,which typically requires the chemical hydrolysis of the hazardous LiO_(2)or Li_(2)O_(2)intermediate,posing risks to the battery ***,we report a direct 4e–electrochemical approach to LiOH enabled by a single atom catalyst(SAC)consisting of CoN_(3)moieties embedded in graphene(CoN_(3)-G),while Li_(2)O_(2)is formed on the metal-free nitrogen-doped graphene(NG).The direct 4e–LiOH pathway significantly reduces the parasitic reactions,resulting in negligible damage to the electrolyte and *** stands in strong contrast to the conventional 2e–Li_(2)O_(2)pathway mediated by NG and the indirect LiOH pathway by MnO_(2).Theoretical calculations further clarify that the presence of CoN_(3)sites enhances the adsorption of oxygen-containing intermediates like*OLiO and*Li_(2)O_(2),promoting the protonation of*Li_(2)O_(2)and the cleavage of the O–O bond to form *** work demonstrates a promising strategy to modulate the reaction pathways in LOBs and broadens the applications of SACs.

关键词： single atom catalyst LiOH Li-O_(2)batteries direct 4-electron oxygen reduction pathway selectivity

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Manipulating guest-responsive spin transition to achieve switchable fluorescence in a Hofmann-type framework

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Science China chemistry 2024年第10期67卷 3339-3346页

作者： Xue-Ru Wu Shu-Qi Wu Zhi-Kun Liu Ming-Xing Chen Jun Tao Osamu Sato Hui-Zhong Kou engineering research center of advanced Rare Earth Materials(ministry of education) Department of ChemistryTsinghua UniversityBeijing 100084China Institute for Materials chemistry and engineering&IRCCS Kyushu University744 MotookaNishi-kuFukuoka 819-0395Japan Key Laboratory of Cluster Science of ministry of education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China Analytical Instrumentation center College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The change of fluorescence emission manipulated by spin state transition attracts considerable attention owing to its potential applications in magneto-optical switching ***,we report two two-dimensional(2D)Hofmann-type spin crossover(SCO)metal-organic frameworks(MOFs)[Fe^(Ⅱ)(PNI)_(2){Ag^(Ⅰ)(CN)_(2)}_(2)]·CHCl_(3)(3Ag·CHCl_(3))and[FeⅡ(PNI)_(2){AuⅠ(CN)_(2)}_(2)]·CHCl_(3)(3Au·CHCl_(3))based on the fluorescent ligand N-(4-pyridylmethyl)-1,8-naphthalimide(PNI).Both complexes exhibit interesting SCO behaviors switched by guest solvent molecules,namely three-step transitions for the solvated complexes and complete onestep hysteretic SCO for the desolvated ones,verified by temperature-dependent magnetic susceptibility measurements,Mossbauer spectra,structural analyses,and differential scanning calorimetry ***,temperature-dependent fluorescence spectra exhibit double peaks(monomer and excimer emission)with both emission peaks change consistent with the change in SCO properties during the solvent molecule *** this study,we integrated guest-responsive SCO behavior into MOFs to manipulate the multistability of spin state and fluorescence switching,providing a rational strategy for the development of stimuli-responsive multifunctional materials.

关键词： spin crossover fluorescence multifunctional materials metal-organic frameworks Hofmann-type

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Zeolites for the separation of ethylene,ethane,and ethyne

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Frontiers of chemical Science and engineering 2024年第9期18卷 137-146页

作者： Binyu Wang Qiang Li Haoyang Zhang Jia-Nan Zhang Qinhe Pan Wenfu Yan State Key Laboratory of Inorganic Synthesis&Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Key Laboratory of advanced Energy catalytic and Functional Materials Preparation College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450012China Key Laboratory of advanced Materials of Tropical Island Resources(ministry of education) School of Chemistry and Chemical EngineeringHainan UniversityHaikou 570228China

The cost-effective separation of ethylene(C_(2)H_(4)),ethyne(C_(2)H_(2)),and ethane(C_(2)H_(6))poses a significant challenge in the contemporary chemical *** contrast to the energy-intensive high-pressure cryogenic distillation process,zeolite-based adsorptive separation offers a low-energy *** review provides a concise overview of recent advancements in the adsorptive separation of C_(2)H_(4),C_(2)H_(2),and C_(2)H_(6)using zeolites or zeolite-based *** commences with an examination of the industrial significance of these compounds and the associated separation ***,it systematically examines the utilization of various types of zeolites with diverse cationic species in such separation *** then it explores how different zeolitic structures impact adsorption and separation capabilities,considering principles such as cation-πinteraction,π-complexation,and steric separation concerning C_(2)H_(4),C_(2)H_(2),and C_(2)H_(6)***,it discusses methods to enhance the separation performance of zeolites and zeolite-based adsorbents,encompassing structural design,modifications,and ion exchange ***,it summarizes current research trends and future directions,highlighting the potential application value of zeolitic materials in the field of C_(2)H_(4),C_(2)H_(2),and C_(2)H_(6)separation and offering recommendations for further investigation.

关键词： zeolite ethylene ethane cation-πinteraction π-complexation

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MXenes/CNTs-based hybrids:Fabrications,mechanisms,and modification strategies for energy and environmental applications

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Nano research 2024年第5期17卷 3429-3454页

作者： Jizhou Jiang Fangyi Li Lei Ding Chengxun Zhang Arramel Xin Li School of Environmental Ecology and Biological engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Nano center Indonesia Jl.PUSPIPTEK Tangerang SelatanBanten 15314Indonesia Institute of Biomass engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

Emerging two-dimensional(2D)layered metal carbide and nitride materials,commonly termed MXenes,are increasingly recognized for their applications across diverse fields such as energy,environment,and *** the past few years,MXenes/carbon nanotubes(CNTs)-based hybrids have attracted extensive attention as an important catalyst in energy and environmental fields,due to their superior multifunctions and mechanical *** review aims to address the fabrication strategies,the identification of the enhancement mechanisms,and recent progress regarding the design and modification of MXenes/CNTs-based hybrids.A myriad of fabrication techniques have been systematically summarized,including mechanical mixing,spray drying,three-dimensional(3D)printing,self-assembly/in-situ growth,freeze drying,templating,hydrothermal methods,chemical vapor deposition(CVD),and ***,the identification of the enhancement mechanisms was thoroughly discussed from the two dimensions of theoretical simulations and in-situ ***,the recent advancements in profound applications of MXenes/CNTs-based hybrids have also been carefully revealed,including energy storage devices,sensors,water purification systems,and microwave *** also underscore anticipated challenges related to their fabrication,structure,underlying mechanisms,modification approaches,and emergent ***,this review offers insights into prospective directions and the future trajectory for these promising *** is expected that this review can inspire new ideas or provide new research methods for future studies.

关键词： MXenes/carbon nanotubes(CNTs)-based hybrids fabrication applications modification strategies

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