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Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

Journal of Energy chemistry 2024年第3期90卷 7-15,I0002页

作者： Ruixue Zheng Qinglei Meng Hao Zhang Teng Li Di Yang Li Zhang Xiaolong Jia Changpeng Liu Jianbing Zhu Xiaozheng Duan Meiling Xiao Wei Xing State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air *** Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active *** by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) *** a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N *** from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(*** hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 *** dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR *** situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C *** work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

关键词： Fe single atom catalysts Oxygen reduction reaction Mesoporous structure Active sites Zinc-air battery

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Recent progress in photocatalytic NAD(P)H regeneration for photocatalytic-enzymatic-coupling system

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 1-24页

作者： Wei Lan Maodi Wang Huicong Dai Qihua Yang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Zhejiang Key Laboratory for Reactive Chemistry on Solid SurfacesInstitute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

The enzymatic redox reactions in natural photosynthesis rely much on the participation of cofactors,with reduced nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate(NADH/NADPH)or their oxidized form(NAD+/NADP+)as an important redox *** photocatalytic regeneration of expensive and unstable NADH/NADPH in vitro is an important process in enzymatic reduction and has attracted much research *** different types of photocatalysts have been developed for photocatalytic NADH/NADPH regeneration,the efficiency is still relatively *** elucidate the key factors affecting the performance of photocatalytic NADH/NADPH regeneration is helpful to rationally design the photocatalyst and improve the photocatalytic *** this paper,we overview the recent progress in photocatalytic NADH/NADPH regeneration with the focus on the strategies to improve the visible light adsorption,the charge separation and migration efficiency,as well as the surface reaction,which jointly determine the overall photocatalytic regeneration *** potential development of photocatalytic NADH/NADPH regeneration and photocatalyticenzymatic-coupling system is prospected finally.

关键词： photocatalytic-enzymatic coupling NAD(P)H regeneration photocatalysis efficiency

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Molecular Chain Flexibility and Dielectric Loss at High-Frequency:Impact of Ester Bond Arrangement in Poly(ester imide)s

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Chinese Journal of Polymer Science 2024年第8期42卷 1122-1133页

作者： Ya-Dong Li Hong Li Lu-Kun Feng Feng Bao Ming-Liang Wang Cai-Zhen Zhu Zhao-Hui Zheng Xiao-Bin Ding Jian Xu Chengdu institute of Organic chemistry Chinese Academy of SciencesChengdu 610041China University of Chinese Academy of Sciences Beijing 100081China institute of Low-Dimensional Materials Genome Initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

The evolution of high-frequency communication has accentuated the significance of controlling dielectric properties in polymer ***,it has been theorized that rigid molecular chains lead to lower dielectric ***,the validity of this proposition at high frequencies remains *** scrutinize the correlation between chain flexibility and dielectric properties,we synthesized six poly(ester imide)s(PEIs)with systematically varied molecular chain flexibilities by modifying the ester's substitution on the aromatic *** introduction of ester bonds bestowed all PEI films with a low dielectric dissipation factor(D_(f)),ranging from 0.0021 to 0.0038 at 10 GHz in dry *** dry D_(f)displayed a pattern consistent with volume polarizability(P/V).Unexpectedly,PI-mmm-T,featu ring the most flexible molecular chain,exhibited the lowest dielectric loss under both dry(0.0021@10 GHz)and hygroscopic(0.0029@10 GHz)***,the observed increase in D_(f)after humidity absorption suggests that the high dielectric loss of PEI in applications may be attributed to its hygroscopic *** simulations and characterization of the aggregation structure revealed that the smaller cavities within flexible molecular chains,after close stacking,impede the entry of water *** sacrificing high-temperature resistance,the precursor exhibited enhanced solubility properties and could be processed into high-quality *** research unveils new insights into the relationship between flexibility and highfrequency dielectric loss,offering innovative perspectives on synthesizing aromatic polymers with exceptional dielectric properties.

关键词： 5G communications Poly(ester imide)s Molecular chain flexibility Dielectric properties Humidity absorption

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Polyoxometalate as the assembly material to self-assembled Ni(OH)_(2)nanosheets with electrocatalytic performance

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Nano Research 2024年第8期17卷 7061-7067页

作者： Danyang He Tianyang Li Luozhen Jiang Fei Wang Zihao Xing Nan Wang Zhiyu Jia Guo-Yu Yang Key Laboratory of Cluster Science Ministry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Shanghai Advanced Research institute Chinese Academy of ScienceShanghai 201210China Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Facluty of ChemistryNortheast Normal UniversityChangchun 130024China

Developing non-noble metal-based electrocatalyst with high catalytic activity is essential for advancing hydrogen energy *** study introduces a hydrothermal method for synthesizing order Ni(OH)_(2)nanosheets,with H_(3)O_(40)PW_(12)(denoted as PW_(12))loaded onto reduced graphene oxide(rGO)coated on nickel foam(referred to as PW_(12)-Ni(OH)_(2)/rGO).This method contrasts with the electrodeposition of Ni(OH)_(2),where PW_(12)is added to the synthetic system to direct the assembly and morphology of the Ni(OH)_(2)through a hydrothermal *** this work,the nickel foam acts dual roles as both the substrate and the source of nickel for the formation of Ni(OH)_(2).The PW_(12)-Ni(OH)_(2)/rGO nanosheets,when successfully prepared and loaded onto the nickel foam(NF),exhibited superior electrocatalytic activity for the hydrogen evolution reaction(HER)in an alkaline electrolyte,achieving a current density of 10 mA·cm^(-2)at an overpotential of 69 ***,we endeavored to expand the application of this material towards the oxygen evolution reaction(OER)by preparing PW_(12)-(Fe/Co)Ni(OH)_(2)/rGO through the addition of metal *** nanocomposite displayed outstanding electrocatalytic activity in alkaline electrolytes,with a current density of 10 mA·cm^(-2)at an overpotential of 211 mV,and demonstrated excellent stability over a 50 h period in a 1 M KOH *** results presented in this paper offer an effective strategy for the preparation of polyoxometalate-based inorganic materials with diverse functionalities,applicable to both HER and OER.

关键词： polyoxometalate Ni(OH)_(2) assembly hydrogen evolution reaction oxygen evolution reaction

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Defect engineering of W^(6+)-doped NiO for high-performance black smart windows

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Nano Research 2024年第4期17卷 3043-3052页

作者： Yingjun Xiao Xiang Zhang Dukang Yan Jianbo Deng Mingjun Chen Hulin Zhang Wenhai Sun Jiupeng Zhao Yao Li School of chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001China Center for Composite Materials and Structure Harbin Institute of TechnologyHarbin 150001China

In this report,W^(6+)doping as a defect engineering strategy has been proposed to improve the electrochromic properties of NiO *** research was conducted to explore the electrochromic properties and the modified mechanism of W-doped NiO *** to the pure NiO,W-doped NiO film exhibits improved electrochromic properties with significant optical modulation(61.56%at 550 nm),fast switching speed(4.42 s/1.40 s for coloring/bleaching),high coloration efficiency(45.41 cm^(2)·C-1)and outstanding cycling stability(no significant attenuation after 2000 cycles)in Li-based *** functional theory(DFT)calculations combined with the experimental results indicate that the improved electrochromic properties were due to enhanced the electronic conductivity and ion conductivity after the introduction of W^(6+).The charge capacity of W-doped NiO has also been improved,and it can function with WO_(3) to achieve a high performance black electrochromic smart window(ECSW)by balancing *** work could advance the fundamental understanding of defect engineering as an effective strategy to boost the electrochromic properties of NiO anodic material,manifesting a significant development as a candidate counter electrode in high-performance black smart windows.

关键词： NiO defect engineering charge balance black electrochromic windows

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A Highly Efficient Ni/Al_(2)O_(3)-LaO_(x) Catalyst for the Reductive Amination of Furfural to Furfurylamine:the Promoting Effect of La

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Chemical Research in Chinese Universities 2024年第1期40卷 36-46页

作者： YANG Yinze ZHANG Liyan ZHOU Leilei CHENG Haiyang ZHAO Fengyu State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied chemistry and Engineering University of Science Technology of ChinaHefei 230026P.R.China Jilin Province Key Laboratory of Green chemistry and Process Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China

The reductive amination of furfural to furfurylamine is an important and still challenging topic in the field of biomass conversion. In this work, we prepared a series of Ni/Al_(2)O_(3)-LaO_(x) catalysts by co-precipitation method, the role of La played in promoting the catalytic performances of reductive amination furfural was discussed based on the changes in the electronic state of Ni species, acidity, and Ni particle size. The catalytic activity and the selectivity of furfurylamine are highly dependent on the surface properties and the structure of the catalyst. The addition of La promoted the amount of strong acidic sites and the H2dissociation and spillover on the surface, thus inducing the improvement of the catalytic activity and furfurylamine selectivity. The Ni/Al_(2)O_(3)-0.5LaO_(x)catalyst with suitable acid sites gave a high yield of furfurylamine (94.9%) under mild reaction conditions. Moreover, the catalyst could be recycled five times without significant loss in activity. The Ni/Al_(2)O_(3)-LaO_(x) catalyst is of great promise in the production of amines via reductive amination reaction.

关键词： Reductive amination Furfural Nickel catalyst Furfurylamine Lanthanum

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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

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Hydrodechlorination of trifluoro-trichloroethane to chlorotrifluoroethylene:Revealing the deactivation mechanism and regeneration strategy of Pd-Cu/AC catalyst

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Chinese Journal of Chemical Engineering 2024年第6期70卷 261-268页

作者： Song Tian Yicheng Chen Xiaoyu Wen Bingcheng Li Jian Lu Zile Li Feng Feng Qingtao Wang Qunfeng Zhang Xiaonian Li State Key Laboratory Breeding Base of Green chemistry Synthesis Technology Institute of Industrial Catalysis of Zhejiang University of TechnologyHangzhou 310014China State Key Laboratory of Fluorine&Nitrogen Chemicals Xi'an Modern Chemistry Research InstituteXi'an 710065China

Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly ***,hydrodechlorination catalysts for olefin production often suffer from poor *** Pd/AC catalyst and Pd-Cu/AC catalyst prepared by co-impregnation method exhibited poor stability,Pd-Cu/AC catalyst with CFC-113 conversion dropping to around 37%after 50 h of hydrodechlorination ***-Emmett-Teller,transmission electron microscopy,X-ray photoelectron spectroscopy,and X-ray diffraction of fresh and deactivated Pd/AC catalysts indicate that the deactivation of Pd/AC catalysts is due to high-temperature agglomeration of *** analysis of fresh and deactivated Pd-Cu/AC catalysts using Brunauer-Emmett-Teller,transmission electron microscopy,and thermogravimetric analysis techniques revealed decreased dispersion of active sites,reduced surface area,catalyst aggregation deactivation,and a significant decrease in Cu ***,the results of NH3-TPD revealed that the acid sites of the catalyst increased significantly.X-ray diffraction spectra indicated the formation of new species,basic copper chloride(Cu_(2)(OH)_(3)Cl),during the *** the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst ***,the deactivated catalyst was successfully reactivated using a simple alkaline washing method.

关键词： CFC-113 Hydrodechlorination Chlorotrifluoroethylene Catalyst deactivation

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Stabilizing high-efficiency iridium single atoms via lattice confinement for acidic oxygen evolution

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Nano Research 2024年第4期17卷 2492-2498页

作者： Yibo Wang Jiadong Jiang Zhaoping Shi Hongxiang Wu Jiahao Yang Pengbo Wang Shuai Hou Meiling Xiao Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026.China State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Key Laboratory of Physics and Technology for Advanced Batteries Ministry of EducationCollege of PhysicsJilin UniversityChangchun 130012China

Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined *** optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic *** high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd ***,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.

关键词： lattice confinement iridium single atoms ultralow iridium loading acidic oxygen evolution proton exchange membrane water electrolysis

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Fabrication of Molecularly Imprinted Electrospun Nanofibers with Mono-amidoxime Functional Ligand for Efficient Decontamination of Toxic Organophosphates

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Chinese Journal of Polymer Science 2024年第4期42卷 446-456页

作者： Lan Wang Peng Jiang Ya-Lin Niu Jun-Peng Cao Tian-Ying Guo Key Laboratory of Functional Polymer Materials Ministry of EducationInstitute of Polymer ChemistryCollege of Chemistry and Frontier Science Center for the Creation of New Organic SubstancesNankai UniversityTianjin300071China

There is an urgent imperative to discover practical and efficacious artificial catalysts for the expeditious decontamination of toxic organophosphates. Herein, we propose a novel molecularly imprinted approach utilizing electrospun fiber scaffolds. Specifically, an amidoxime-based functional polymer (PMAOX) has been synthesized, which contains amidoxime groups that can act as nucleophiles and ligands for the formation of catalytic active sites. This polymer was blended with polyacrylonitrile (PAN), a well-processable material, to prepare a nanofiber mat using electrospinning techniques. Then, the amidoxime side groups on fiber surface were further cross-linked after the molecular coordination of templates to complete the molecularly imprinting process. This approach can not only enhance the content of functional molecularly imprinted polymers without affecting structural stability, but also combines surface MI technology to fully expose and leverage the advantages of active sites. The as prepared molecularly imprinted electrospun nanofibers MIF-Zn-PMAOX/PAN-6/4 catalyzes the degradation of paraoxon with a half-life of 32 min, and MIF-Ag-PMAOX/PAN catalyzes the degradation of parathion with a half-life of 18 min. The maximum catalytic rate evidence rate enhancements nearly 3700-fold of the self-hydrolysis. Thus, the mono-amidoxime based molecularly imprinted fibers demonstrate the versatility and superiority as self-detoxifying for organophosphates.

关键词： Organophosphateshydrolysis Electrospinning Molecular imprinting

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