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One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts: A DFT study

Chinese chemical Letters 2024年第4期35卷 544-548页

作者： Tao Ban Xi-Yang Yu Hai-Kuo Tian Zheng-Qing Huang Chun-Ran Chang Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and TechnologyXi'an Jiaotong UniversityXi'an 710049China Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization School of Chemistry and Chemical EngineeringYulin UniversityYulin 719000China

One-step conversion of methane and formaldehyde into ethanol is a 100% atom-efficient process for carbon resources utilization and environment protection but still faces eminent challenges due to the lacking of efficient catalysts. Therefore, developing active and stable catalysts is crucial for the co-conversion of methane and formaldehyde. Herein, twelve kinds of “Single-Atom”-“Frustrated Lewis Pair”(SA-FLP)dual-active-site catalysts are designed for the direct conversion of methane and formaldehyde to ethanol based on density functional theory(DFT) calculations and microkinetic simulations. The results show that the SA-FLP dual active sites can simultaneously activate methane at the SA site and activate formaldehyde at the FLP site. Among the twelve designed SA-FLP catalysts, Fe1-FLP shows the best performance in the co-conversion of methane and formaldehyde to ethanol with the rate-determining barrier of 1.15 e *** is proved as the main product with the turnover frequency of 1.32 × 10^(-4)s^(-1)at 573 K and 3 *** work provides a universal strategy to design dual active sites on metal oxide materials and offers new insights into the effective conversion of methane and formaldehyde to desired C_(2) chemicals.

关键词： Single-atom Frustrated Lewis pairs Methane conversion Dual active sites Ethanol synthesis

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Ni/Co bimetallic organic frameworks nanospheres for highperformance electrochemical energy storage

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Nano Research 2024年第6期17卷 5122-5130页

作者： Jianru Guan Minlu Liu Limin Zhu Jiamei Wang Qing Han Xiaoxia Yang Weibo Hua Lingling Xie Xiaoyu Cao School of Chemistry and Chemical Engineering Key Laboratory of High Specific Energy Materials for Electrochemical Power Sources of Zhengzhou CityHenan University of TechnologyZhengzhou 450001China School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China School of Environmental Engineering Henan University of TechnologyZhengzhou 450001China

In addition to their many well-known advantages(e.g.,ultra-high porosity,good pore size distribution,easy functionalization,and structural tolerability),metal-organic frameworks(MOFs)are a new class of advanced functional ***,their backbones are highly susceptible to deformation after exposure to acidic or alkaline *** a result of lithium-ion batteries embedding or detaching directly from MOFs,they irreversibly *** a result,they fail to maintain their electrochemical *** factors have hindered the development of MOFs as direct electrode materials,making the design of MOF materials with controlled morphology and stable dimensions a new *** this study,we adopted a versatile and effective method to synthesize a novel MOF material(NiCo-BP(BP=BTC/phen and BTC=1,3,5-benzenetricarboxylic acid))using the rigid ligands 1,10-phenanthroline and homobenzotrizoic acid,and the emergence of the Ni-O/N and Co-O/N coordination layers was observed by extended X-ray absorption fine structure(EXAFS)tests,indicating that Ni and Co were coordinated with heterocyclic N-given atoms to form a stable p-πconjugated ***,the metal-ion is attached to the carboxylic acid ligand on the other side,making the metal-organic skeleton complete and *** nanosphere structure of NiCo-BP(~400 nm)allows for full exposure and utilisation of the active sites,especially the Ni,Co,and phenanthroline units,and exhibit impressively high specific capacity and cycling *** a high current density of 1.0 A·g^(−1),a high discharge specific capacity of 631.6 mAh·g^(−1)was obtained after 1000 *** co-participation of two organic ligands in the coordination is in accordance with the theory of soft and hard acids and bases,which contributes to the ability of the material to maintain a high capacity in cycling as well as its cyclic stability.

关键词： lithium-ion batteries metal organic frame electrochemical energy storage dual ligand hard-soft-acid-base

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Post-treatment of Ti-MWW zeolite with potassium fluoride for propylene epoxidation

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Frontiers of chemical Science and engineering 2024年第8期18卷 37-47页

作者： Xintong Li Xianchen Gong Jilong Wang Shengbo Jin Hao Xu Peng Wu State Key Laboratory of Petroleum Molecular&Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China

Epoxidation of propylene to propylene oxide(PO)with hydrogen peroxide(HPPO)is an environmentally friendly and cost-efficient process in which titanosilicates are used as ***-MWW is a potential industrial catalyst for this process,which involves the addition of HPPO to *** silanol groups generated during secondary crystallization unavoidably result in ring-opening of PO and inefficient decomposition of HPPO,which diminish the PO selectivity and the lifespan of *** address this issue,we conducted post-treatment modifications of the structured Bf-Ti-MWW catalyst with potassium fluoride aqueous *** quenching the silanol groups with potassium fluoride and implanting electron-withdrawing fluoride groups into the Ti-MWW framework,both the catalytic activity and HPPO utilization efficiency were ***,the ring opening reaction of PO was *** a continuous fixed-bed liquid-phase propylene epoxidation reaction,the KF-treated structured Ti-MWW catalyst displayed an exceptionally long lifespan of 2700 h,with a PO yield of 590 g·kg^(-1)·h^(-1).

关键词： titanosilicates Ti-MWW propylene epoxidation structured catalyst KF modification

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Biological Interaction and Imaging of Ultrasmall Gold Nanoparticles

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Nano-Micro Letters 2024年第3期16卷 69-98页

作者： Dongmiao Sang Xiaoxi Luo Jinbin Liu Key Laboratory of Functional Molecular Engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China

Ultrasmall gold nanoparticles(AuNPs)typically includes atomically precise gold nanoclusters(AuNCs)and AuNPs with a core size below 3 *** as a bridge between small molecules and traditional inorganic nanoparticles,the ultrasmall AuNPs show the unique advantages of both small molecules(e.g.,rapid distribution,renal clearance,low non-specific organ accumulation)and nanoparticles(e.g.,long blood circulation and enhanced permeability and retention effect).The emergence of ultrasmall AuNPs creates significant opportunities to address many challenges in the health field including disease diagnosis,monitoring and *** the nano–bio interaction dictates the overall biological applications of the ultrasmall AuNPs,this review elucidates the recent advances in the biological interactions and imaging of ultrasmall *** begin with the introduction of the factors that influence the cellular interactions of ultrasmall *** then discuss the organ interactions,especially focus on the interactions of the liver and *** further present the recent advances in the tumor interactions of ultrasmall *** addition,the imaging performance of the ultrasmall AuNPs is summarized and ***,we summarize this review and provide some perspective on the future research direction of the ultrasmall AuNPs,aiming to accelerate their clinical translation.

关键词： Ultrasmall gold nanoparticle Cellular interaction Organ interaction Tumor interaction Bioimaging

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Upcycling of polyphenylene oxide into 2,6-dimethyl aniline via depolymerization and amination over a Pt/CeO_(2) catalyst

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Science China Chemistry 2025年第2期68卷 520-525页

作者： Shengchao Jia Wenke Zhao Xiaohui Liu Yong Guo Yanqin Wang State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Key Laboratory of Functional Materials Chemistry School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

Upcycling of plastic waste into N-containing compound is a novel and attractive strategy for its disposal and will opens up a promising direction for the production of value-added ***,an efficient strategy for the depolymerization-amination of polyphenylene oxide(PPO)into 2,6-dimethyl aniline is developed over a simple Pt/CeO_(2) *** C–O linkages of PPO can be selectively broken,producing 2,6-dimethyl phenol and then hydrogenated and aminated to 2,6-dimethyl cyclohexylamine over the Pt/CeO_(2) ***,2,6-dimethyl aniline was produced with high selectivity through the dehydrogenation of 2,6-dimethyl cyclohexylamine in the same *** can be used as the hydrogen-acceptor in the dehydrogenation step and enhance the selectivity of target *** N-containing compound,2,6-dimethyl aniline,is obtained and separated after HCl ***,the Pt/CeO_(2) catalyst exhibit remarkable stability and can sustainably catalyze the synthesis of 2,6-dimethyl aniline in several cycles.

关键词： PPO depolymerization-amination 2,6-dimethyl aniline Pt/CeO_(2)

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Simultaneous generation of electricity, ethylene and decomposition of nitrous oxide via protonic ceramic fuel cell membrane reactor

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Journal of Energy Chemistry 2023年第2期77卷 359-368,I0010页

作者： Song Lei Ao Wang Guowei Weng Ying Wu Jian Xue Haihui Wang Guangdong Provincial Key Lab of Green Chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640GuangdongChina Beijing Key Laboratory for Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006GuangdongChina

Ethylene,one of the most widely produced building blocks in the petrochemical industry,has received intense *** production,using electrochemical hydrogen pump-facilitated nonoxidative dehydrogenation of ethane(NDE)to ethylene,is an emerging and promising route,promoting the transformation of the ethylene industry from energy-intensive steam cracking process to new electrochemical membrane reactor *** this work,the NDE reaction is incorporated into a BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(3-δ)electrolyte-supported protonic ceramic fuel cell membrane reactor to co-generate electricity and ethylene,utilizing the Nb and Cu doped perovskite oxide Pr_(0.6)Sr_(0.4)Fe_(0.8)Nb_(0.1)Cu_(0.1)O_(3-δ)(PSFNCu)as anode catalytic *** to the doping of Nb and Cu,PSFNCu was endowed with high reduction tolerance and rich oxygen vacancies,showing excellent NDE catalytic *** maximum power density of the assembled reactor reaches 200 mW cm^(-2)at 750℃,with high ethane conversion(44.9%)and ethylene selectivity(92.7%).Moreover,the nitrous oxide decomposition was first coupled in the protonic ceramic fuel cell membrane reactor to consume the permeated *** a result,the generation of electricity,ethylene and decomposition of nitrous oxide can be simultaneously obtained by a single ***,the maximum power density of the cell reaches 208 mW cm^(-2)at 750℃,with high ethane conversion(45.2%),ethylene selectivity(92.5%),and nitrous oxide conversion(19,0%).This multi-win technology is promising for not only the production of chemicals and energy but also greenhouse gas reduction.

关键词： Nonoxidative dehydrogenation of ethane Ethylene Nitrous oxide decomposition Protonic ceramic fuel cell membrane reactor Perovskite oxide

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Cubic S/N co-doped TiO_(2) with rich oxygen vacancies from Ti-MOFs for efficient elimination of formaldehyde

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Chinese chemical Letters 2024年第2期35卷 512-515页

作者： Qing Gao Lei Sun Zhihua Wang Jiguang Deng State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaDepartment of Chemical EngineeringBeijing University of TechnologyBeijing 100124China

The cubic S/N co-doped TiO_(2)(TNSx,x is the calcination temperature)photocatalysts with rich oxygen vacancies were obtained by high temperature calcination of sulfur powder and titanium-based MOFs NH_(2)-MIL-125 for the photocatalytic removal of gaseous formaldehyde(a volatile organic compound).Among the obtained catalysts,the presence of oxygen vacancies restricted photogenerated electron and holes recombination.98.00%removal of gaseous formaldehyde in 150 min could be achieved over TNS600 by xenon *** removal efficiency for formaldehyde was well retained for five cycle *** results from PL,TRPL and EIS revealed that TNS600 had the best separation efficiency of photogenerated electrons and holes,and the enhanced charge separation led to a significant increase in photocatalytic *** photocatalytic oxidation mechanism indicated that the ^(•)OH and ^(•)O_(2)−radicals were mainly involved in the efficient elimination of gaseous formaldehyde and were able to mineralize formaldehyde to H_(2)O and CO_(2).

关键词： Metal-organic frameworks Photocatalysis Formaldehyde removal S/N co-doped TiO_(2) Oxygen vacancies

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A new 4-Ti-added polyoxometalate

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Tungsten 2024年第2期6卷 465-471页

作者： Hai-Lou Li Chen Lian Guo-Yu Yang MOE Key Laboratory of Cluster Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

A new inorganic–organic hybrid 4-Ti-added polyoxometalate:[H_(2)N(CH_(3))_(2)]_(2)Na_(3)H_(5)[{Ti(C_(2)O_(4))(H_(2)O)}_(2){Ti(C_(2)O_(4))}_(2)(B-β-SbW_(9)O_(33))_(2)]·22H_(2)O(1)has been successfully made and further characterized by infrared spectroscopy,thermogravimetric analysis,powder X-ray diff raction and single-crystal X-ray diff *** polyoxoanion of 1 exhibits a Krebs-type structure that is constructed from two[B-β-SbW_(9)O_(33)]^(9)−fragments fused together by a belt of four additional Ti atoms decorated by oxalate ***,1 as a heterogeneous catalyst exhibits high activity for Knoevenagel condensation under mild reaction conditions.

关键词： Polyoxometalate Ti-added POM Krebs-type structure Knoevenagel condensation

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Controlling of coordination state of Ru_(x)N_(y) clusters for efficient oxygen reduction electrocatalysis

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Nano Research 2024年第3期17卷 1035-1041页

作者： Weiyang Fu Yihuan Yu Tongtong Liu Yinliang Cao Zhengping Zhang Feng Wang State Key Laboratory of Chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology for MaterialsBeijing University of Chemical TechnologyBeijing 100029China Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Zhejiang Tianneng Hydrogen Energy Technology Co. Ltd.Huzhou 313100China

Ruthenium(Ru)is an attractive potential alternative to platinum as an electrocatalyst for the oxygen reduction reaction(ORR),in virtue of its high catalytic selectivity and relatively low *** this work,a series of well-dispersed nitrogen-coordinated Ru-clusters on carbon black(Ru_(x)N_(y)/C)were prepared by pyrolyzing different Ru-containing sandwich compounds as the Ru *** higher thermal stability of these complexed sandwich precursors(bis(1,2,3,4,5-pentamethylcyclopentadienyl)Ru(II)monomer,dichloro(p-cymene)Ru(II)dimer,and chloro(1,2,3,4,5-pentamethylcyclopentadienyl)Ru(II)tetramer)affords the control of coordinated state for the resulting Ru-clusters,in comparison of that derived from ruthenium *** the pyrolysis treatment,the Ru coordinated state in Ru_(x)N_(y)/C,with the Ru–N and Ru–Ru bonds,still showed the structural inheritance from the Ru(II)monomer,dimer,and tetramer,but using ruthenium chlorides as the Ru source resulted in the nanoscale Ru *** ORR testing exhibited that the Ru_(x)N_(y)/C sample derived from the Ru(II)tetramer(Ru_(x)N_(y)/C-T)presents the higher catalytic activity than the other obtained samples in either alkaline or acidic *** in the acidic electrolyte,Ru_(x)N_(y)/C-T shows the comparable ORR activity to that of Pt/C catalysts,and it shows the superior tolerance against methanol and *** X-ray absorption spectroscopy and density functional theory calculations demonstrate that these tetra-nuclear Ru-clusters could be the most active site due to their broadened d-orbital bands and lower energy d-band center than those of other subnano species and nanocrystals,and their favorable Yeager-type adsorption of O_(2)-molecules is also contributed to promoting O–O bond cleavage and accelerating the ORR process.

关键词： ruthenium clusters coordination environment sandwich compounds electrocatalysis oxygen reduction reaction

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Modulating electronic structure of nickel diselenide by vanadium doping toward highly efficient and stable bifunctional electrocatalysts for overall water splitting

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Journal of Materials Science & technology 2024年第20期187卷 63-71页

作者： Miaomiao Bai Taotao Ai Weiwei Bao Jie Han Junjun Zhang Qi Yu Jiangying Liu Xueling Wei Xiangyu Zou Liangliang Feng National and Local Joint Engineering Laboratory for Slag Comprehensive Utilization and Environmental Technology School of Materials Science and EngineeringShaanxi University of TechnologyHanzhong 723000China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry&Chemical EngineeringNingxia UniversityYinchuan 750021China School of Materials Science&Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science&TechnologyXi’an 710021China

Designing low-cost and high-efficiency bifunctional electrocatalysts is one of the challenges in the clean production of hydrogen energy in electrochemical water *** metal selenides(TMSes)have been widely studied because of their low price,intrinsic metal properties,and high catalytic *** addition,the synergistic effect between bimetallic selenides exhibits better performance than monometallic selenides in the electrocatalytic ***,we synthesized V-doped NiSe2 nanowire arrays on pretreated nickel foam by a convenient two-step hydrothermal synthesis *** the al-kaline electrolyte,V-NiSe_(2)/NF exhibited excellent OER catalytic activity(293.6 mV@50 mA cm^(-2)).In ad-dition,the introduction of heteroatom V induces stronger electronic interactions between the structural atoms of the catalyst,altering the electronic structure and causing V-NiSe_(2)/NF to demonstrate excellent OER *** the long-term OER test,V-NiSe_(2)/NF was converted into NiOOH and SeO_(x)^(2-),which may be the“real”active species during catalytic reactions,and we also successfully captured the for-mation of intermediate NiOOH and selenite as active centers in the OER process through in-situ *** theoretical calculation shows that the electron transfer modulates the electron structure,changes the adsorption-desorption energy of the reaction intermediates,reduces the potential barrier of the rate-limiting step,and improves the OER *** V doping engineering strategy and the unique nanowire array structure make TMSes exhibit excellent OER *** study provides a new idea for the design of TMSe catalysts with excellent electrocatalytic performance.

关键词： Electrocatalysis Oxygen evolution reaction Vanadium doping Overall water splitting In-situ Raman Density functional theory

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