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Recent advances in cobalt phosphide-based materials for electrocatalytic water splitting:From catalytic mechanism and synthesis method to optimization design

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Nano Materials Science 2024年第2期6卷 139-173页

作者： Rongrong Deng Mengwei Guo Chaowu Wang Qibo Zhang Key Laboratory of Ionic Liquids Metallurgy Faculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming650093PR China State Key Laboratory of Complex Nonferrous Metal Resources Cleaning Utilization in Yunnan Province Kunming650093PR China

Electrochemical water splitting has long been considered an effective energy conversion technology for trans-ferring intermittent renewable electricity into hydrogen fuel,and the exploration of cost-effective and high-performance electrocatalysts is crucial in making electrolyzed water technology commercially *** phosphide(Co-P)has emerged as a catalyst of high potential owing to its high catalytic activity and durability in water *** paper systematically reviews the latest advances in the development of Co-P-based materials for use in water *** essential effects of P in enhancing the catalytic performance of the hydrogen evolution reaction and oxygen evolution reaction are first ***,versatile synthesis techniques for Co-P electrocatalysts are summarized,followed by advanced strategies to enhance the electrocatalytic performance of Co-P materials,including heteroatom doping,composite construction,integration with well-conductive sub-strates,and structure control from the viewpoint of *** with these optimization strategies,the understanding of the inherent mechanism of enhanced catalytic performance is also ***,some existing challenges in the development of highly active and stable Co-P-based materials are clarified,and pro-spective directions for prompting the wide commercialization of water electrolysis technology are proposed.

关键词： Co-P electrocatalysts Water splitting Hydrogen production catalytic mechanism Synthesis technique Optimization design

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The hydrogen storage performance and catalytic mechanism of theMgH_(2)-MoS_(2)composite

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镁合金学报(英文) 2023年第7期11卷 2530-2540页

作者： Luxiang Wang Yiwanting Hu Jiayu Lin Haiyan Leng Chenghua Sun Chengzhang Wu Qian Li Fusheng Pan State Key Laboratory of Advanced Special Steel&Shanghai Key Laboratory of Advanced Ferrometallurgy&School of Materials Science and Engineering Shanghai UniversityShanghai 200444China Centre for Translational Atomaterials Faculty of ScienceEngineering and TechnologySwinburne University of TechnologyHawthornVictoria 3122Australia National Engineering Research Center for Magnesium Alloys College of Materials Science and EngineeringChongqing UniversityChongqing 400044China

In this work,we synthesized MoS_(2)catalyst via one-step hydrothermal method,and systematically investigated the catalytic effect of MoS_(2)on the hydrogen storage properties of MgH_(2).The MgH_(2)-5MoS_(2)composite milled for 5 h starts to release hydrogen at 259℃.Furthermore,it can desorb 4.0 wt.%hydrogen within 20 min at 280℃,and absorb 4.5 wt.%hydrogen within 5 min at 200℃.Mo and MoS_(2)coexistedin the ball milled sample,whereas only Mo was kept in the sample after dehydrogenation and rehydrogenation,which greatly weakens theMg-H bonds and facilitates the dissociation of MgH_(2)on the surface of Mo(110).The comparative study show that the formed MgS has nocatalytic effect for MgH_(2).We believed that the evolution and the catalytic mechanism of MoS_(2)will provide the theoretical guidance for theapplication of metal sulfide in hydrogen storage materials.

关键词： Hydrogen storage Magnesium hydride MoS_(2) Evolution catalytic mechanism

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Structural insights into the catalytic mechanism of aldehyde-deformylating oxygenases

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Protein & Cell 2015年第1期6卷 55-67页

作者： Cheniun Jia Mei Li Jianjun Li Jingjing Zhang Hongmei Zhang Peng Cao Xiaowei Pan Xuefeng LU Wenrui Chang National Laboratory of Biomacromolecules Institute of Biophysics Chinese Academy of Sciences Beijing 100101 China Key Laboratory ofBiofuels Shandong Provincial Key Laboratory of Energy Genetics Qingdao Instituie of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 China University of Chinese Academy of Sciences Beijing 100049 China

The fatty alk（a/e）ne biosynthesis pathway found in cyanobacteria gained tremendous attention in recent years as a promising alternative approach for biofuel production. Cyanobacterial aldehyde-deformylating oxygenase （cADO）, which catalyzes the conversion of Cn fatty aldehyde to its corresponding Cn-1 alk（ale）ne, is a key enzyme in that pathway. Due to its low activity, alk（a/e）ne production by cADO is an inefficient process. Previous biochemical and structural investi. gations of cADO have provided some information on its catalytic reaction. However, the details of its cata- lytic processes remain unclear. Here we report five crystal structures of cADO from the Synechococcus elongates strain PCC7942 in both its iron-free and iron-bound forms, representing different states during its catalytic process. Structural comparisons and functional enzyme assays indicate that Giu144, one of the iron-coordinating residues, plays a vital role in the catalytic reaction of cADO. Moreover, the helix where Glu144 resides exhibits two distinct conformations that correlates with the different binding states of the di-iron center in cADO structures. Therefore, our results provide a structural explanation for the highly labile feature of cADO di-iron center, which we pro- posed to be related to its low enzymatic activity. On the basis of our structural and biochemical data, a possible catalytic process of cADO was proposed, which could aid the design of cADO with improved activity.

关键词： aldehyde-deformylating oxygenase di-ironcenter crystal structure catalytic mechanism alk(a/e)neproduction

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Revealing the catalytic mechanism of an ionic liquid with an isotope exchange method

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Petroleum Science 2011年第4期8卷 495-501页

作者： Sun Xuewen Zhao Suoqi State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing 102249 China

The alkylation mechanism catalyzed by an ionic liquid （as a Lewis acid） may be different from the traditional alkylation mechanism catalyzed by Br nsted acid,especially as their initiation steps are still not *** this paper,an isotope exchange method is used to investigate the catalytic mechanism of AlCl 3 /butyl-methyl-imidazolium chloride ionic liquid in the alkylation of benzene with *** proposed catalytic mechanism was confirmed by analysis of ionic liquid before and after reaction and of the alkylation products of deuterated benzene （C 6 D 6） with *** proposed mechanism consists of the equilibrium reaction between [Al 2 Cl 7 ] ＋H ＋ and [AlHCl 3 ] ＋＋[AlCl 4 ],in which the Br nsted acid [AlHCl 3 ] ＋ is supplied by the reaction of 2-H on the imidazolium ring and [Al 2 Cl 7 ].The alkylation reaction is initiated by the Br nsted acid [AlHCl 3 ] ＋ which reacts with 1-dodecene to form a carbonium ion,then the carbonium ion reacts with benzene to form an unstable σ complex,leading to the formation of 2-phenyldodecane.

关键词： catalytic mechanism ionic liquid isotope exchange method alkylation deuterated benzene

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Valance electron structure of carbide-diamond interface and catalytic mechanism for diamond synthesis under high-pressure and high-temperature

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Progress in Natural Science:Materials International 2006年第8期16卷 852-858页

作者： GONG Jianhong, XU Bin, YIN Longwei, QI Yongxin, LI Li, SU Qingcai and LI Musen (School of Materials Science and Engineering, Shandong University, Jinan 250061, China Department of Materials Science and Engineering, Shandong Institute of Architecture and Technology, Jinan 250014, China Shandong Engineering and Technology Research Center of Super-hard Materials, Zoucheng 273500, China) School of Materials Science and Engineering Shandong University Jinan 250061 China Shandong Engineering and Technology Research Center of Super-hard Materials Zoucheng 273500 China Department of Materials Science and Engineering Shandong Institute of Architecture and Technology Jinan 250014 China

The metallic films surrounding a synthetic diamond formed under high-pressure and high-temperature (HPHT) in the presence of Fe-based and Ni-based catalysts were studied by scanning electron microscopy (SEM), X-ray diffraction (XRD) and transmission electron microscopy (TEM). It was showed that the carbide was the primary carbon source for the nucleation and growth of diamond. Based on the EET (empirical electron theory in solid and molecules) theory, the valence electron structure of interface between carbide (Fe3C, Ni3C, (Fe, Ni)3C) and diamond was calculated using the bonding length difference (BLD) method. The boundary criterion of Thomas-Fermi-Dirac-Cheng (TFDC): "the electron density being equal on the contacting surfaces of atoms" was applied to analyze the valence structure of carbide-diamond interface. The result based on the calculation valance electron structure is in good accordance with the experimental result. This study is very helpful to reveal the catalytic mechanism of diamond nucleation and growth and design the new catalyst for diamond synthesis.

关键词： synthetic diamond carbide catalytic mechanism valence electron theory interface.

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Properties and catalytic mechanism of γ-glutamyltranspeptidase from *** NX-2

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Frontiers of Chemical Science and Engineering 2008年第4期2卷 456-461页

作者： Qian WANG Zhong YAO Zhijing XUN Xiaoying XU Hong XU Ping WEI College of Life Science and Pharmacy Nanjing University of TechnologyNanjing 210009China

Sinceγ-glutamyltranspeptidase(GGT)especially catalyses the transfer of theγ-glutamyl moiety to a variety of amino acids and short peptides,GGT has important practical value for enzymatic synthesis ofγ-glutamyl *** this paper,the GGT produced from Bacillus subtilis NX-2 was purified by a combination of ammonium sulfate fractionation and ion exchange chromatography,and the properties of purified GGT were *** the conditions of pH 10.0,D-glutamine(D-Gln)/L-tryptophan(L-Trp)with a molar ratio of 5:7,a temperature 40℃ and a reaction time of 4 h,a higher conversion rate of 42%was *** to the time course,the catalytic mechanism of enzymatic synthesis ofγ-D-glutamyl-L-tryptophan(γ-D-Gln-L-Trp)was *** was demonstrated that the GGT can catalyze not only the reaction of transpeptidation,but also the irreversible hydrolysis of the products which results in the decrease of the yield of the *** affinity parameter of GGT to D-Gln(Km)was 5.08 mmol·L-1 and the maximum reaction rate of transpeptidation(rmax)was determined as 0.034 mmol·min-1·L-1,while the affinity parameter of GGT toγ-D-Gln-L-Trp(K’m)was 2.267 mmol·L-1,and the maximum reaction rate of hydrolysis(r’max)was 0.012 mmol·min-1·L-1.

关键词： c-glutamyltranspeptidase purification prop-erties c-D-glutamyl-L-Tryptophan catalytic mechanism

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Exceptional catalytic effect of novel rGO-supported Ni-Nb nanocomposite on the hydrogen storage properties of MgH_(2)

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Journal of Materials Science & Technology 2024年第5期172卷 83-93页

作者： Samuel Guemou Liuting Zhang Shuai Li Yiqun Jiang Tao Zhong Zichuan Lu Ren Zhou Fuying Wu Qian Li School of Energy and Power Instrumental Analysis CenterJiangsu University of Science and TechnologyZhenjiang 212003China National Engineering Research Center for Magnesium Alloys&National Key Laboratory of Advanced Casting Technologies&College of Materials Science and Engineering Chongqing UniversityChongqing 400044China Chongqing Institute of New Energy Storage Materials and Equipment Chongqing 401135China Max Planck Institute for Iron Research Düsseldorf 40237Germany

The design of an excellent active catalyst to improve the sluggish kinetic and thermodynamic properties of magnesium hydride(MgH_(2))remains a great challenge to achieve its practical *** this study,a novel Ni-Nb/rGO nanocomposite catalyst was successfully prepared by one-spot hydrothermal and sub-sequent calcination *** novel Ni-Nb/rGO nanocomposite exhibits an exceptional catalytic effect on improving MgH_(2) sorption ***,the onset desorption temperature of MgH_(2)+10 wt%Ni-Nb/rGO composite is reduced to 198℃,much lower than that of undoped MgH_(2)(330℃).In-terestingly,the composite can release 5.0,5.9,and 6.0 wt%H_(2) within 10 min at 245,260,and 275℃,***,the dehydrogenated MgH_(2)+10 wt%Ni-Nb/rGO composite starts to absorb hydrogen even at room temperature with approximate 2.75 wt%H_(2) uptake at 75℃under 3 MPa H_(2) pressure within 30 min and exhibits excellent stability by maintaining 6.0 wt%hydrogen content after 20 cycles at 300℃.Chou’s model suggests that the de/hydrogenation kinetics of Ni-Nb/rGO-modified MgH_(2) switches from surface penetration model to diffusion model at lower ***,the ac-tivation energies(E a)for the de/hydrogenation of MgH_(2)+10 wt%Ni-Nb/rGO are reduced to 57.8 kJ/mol and 33.9 kJ/mol,which are significantly lower than those of undoped MgH_(2).The work demonstrates that the addition of a novel ternary Ni-Nb/rGO catalyst is an effective strategy to not only boost the sorption kinetics of MgH_(2) but also maintain its cycling property.

关键词： Hydrogen storage materials Magnesium hydride Ni-Nb/rGO Kinetic analysis catalytic mechanism

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A review on the chemo-catalytic conversion of cellulose to bio-ethanol

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Green Chemical Engineering 2024年第03期5卷 276-289页

作者： Xiuzheng Zhuang Haiyong Wang Shugen Jiang Xiaohong Hu Tong Su Xinghua Zhang Longlong Ma Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and Environment Southeast University Key Laboratory of Renewable Energy Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Wuzhou Refrigeration Group Co.Ltd.

While the industry has produced sugar-derived ethanol from the conventional method of fermentation for hundreds of years, other effective routes involving the direct transformation of carbohydrates still remain extremely rare. Very recently, an innovative chemo-catalytic method driven by the aqueous-phase catalysis was created for the synthesis of cellulosic ethanol, making a great breakthrough in the common ways as it can theoretically utilize all of the carbon atoms in sugars with faster kinetics; up to now, results from the relevant studies have been accumulated to a certain extent, but the periodic conclusions in this field are unfortunately absent. For this reason,this work tries to offer an overview of the cellulosic ethanol produced by chemo-catalytic routes, highlighting the present knowledge in relation to the technical efficiency, catalytic mechanisms as well as practical applications. At first, the advanced progress on the increasing efficiency from a varied type of catalytic systems are extensively discussed, which involves the specific functions of hybrid components from different strategies; meanwhile, the general influences of processing conditions, such as the hydrothermal severity and aqueous environments, are also identified. Subsequently, possible mechanisms behind the chemo-catalytic processes are widely elaborated by analyzing a number of experimental cases associated with the reaction network and its kinetic models. After that,the actual effects of this technique on the real biomass are collected to identify the positive/negative interactions between multiple components, together with the potential solutions on the semi-continuous processes of pilot scale application. The techno-economic analysis(TEA) is also calculated and compared with other similar methods, such as fermentation and gasification. Finally, several proposals aimed at upgrading the whole chain of chemo-catalytic processes are clearly provided, which may function as a guideline f

关键词： Cellulosic ethanol Chemo-catalytic method Influencing factors catalytic mechanism Techno-economic analysis

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Peroxidase-like active Cu-ZIF-8 with rich copper(I)-nitrogen sites for excellent antibacterial performances toward drug-resistant bacteria

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Nano Research 2024年第8期17卷 7427-7435页

作者： Xiaoze Wang Hui Wang Jingkun Zhang Ning Han Wenjun Ma Donghai Zhang Mingshui Yao Xianliang Wang Yunfa Chen State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of the Chinese Academy of Sciences Beijing 100049China Laboratory of Theoretical and Computational Nanoscience CAS Key Laboratory of Nanosystem and Hierarchial FabricationCAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China China CDC Key Laboratory of Environment and Population Health National Institute of Environmental HealthChinese Center for Disease Control and PreventionBeijing 100021China

Bacterial pathogens pose a serious threat to human health,and there is an urgent need to develop highly effective antibacterial materials to eliminate the increasingly serious contamination of drug-resistant ***,a Cu-doped ZIF-8 particle with unsaturated copper exhibits high peroxidase-like activity.99.998%antibacterial efficiency against *** can be achieved for 30 min at a low concentration of 50μg·mL^(−1),as well as complete sterilization against ***(up to 8 log).99.999%antibacterial efficiency against Methicillin-resistant Staphylococcus aureus can be achieved,performing orders of magnitude higher than *** mechanism shows that the unsaturated Cu-Nx sites are enzyme-like active centers,which could promote the consumption of bacteria reducing substances by H_(2)O_(2),and the generated*OH further aggravates bacterial oxidative stress and membrane *** importantly,the oxidation activity of adsorbed oxygen species on Cu-ZIF-8 is enhanced by charge transfer and structural changes between the ligand and copper center like natural ***-doped ZIF-8 with peroxidase-like activity shows great potential in antibacterial application and the revealed catalytic mechanism is helpful for understanding the high antibacterial activity of nanoparticles with Cu-Nx sites.

关键词： Cu-doped ZIF-8 peroxidase-like reactive oxygen species(ROS) catalytic mechanism antibacterial activity

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Deep Insight of Design,mechanism,and Cancer Theranostic Strategy of Nanozymes

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Nano-Micro Letters 2024年第2期16卷 165-217页

作者： Lu Yang Shuming Dong Shili Gai Dan Yang He Ding Lili Feng Guixin Yang Ziaur Rehman Piaoping Yang Key Laboratory of Superlight Materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001People’s Republic of China Yantai Research Institute Harbin Engineering UniversityYantai 264000People’s Republic of China Key Laboratory of Green Chemical Engineering and Technology of Heilongjiang Province College of Material Science and Chemical EngineeringHarbin University of Science and TechnologyHarbin 150040People’s Republic of China Department of Chemistry Quaid-i-Azam UniversityIslamabad 45320Pakistan

Since the discovery of enzyme-like activity of Fe3O4 nanoparticles in 2007,nanozymes are becoming the promising substitutes for natural enzymes due to their advantages of high catalytic activity,low cost,mild reaction conditions,good stability,and suitable for large-scale ***,with the cross fusion of nanomedicine and nanocatalysis,nanozyme-based theranostic strategies attract great attention,since the enzymatic reactions can be triggered in the tumor microenvironment to achieve good curative effect with substrate specificity and low side ***,various nanozymes have been developed and used for tumor *** this review,more than 270 research articles are discussed systematically to present progress in the past five ***,the discovery and development of nanozymes are ***,classification and catalytic mechanism of nanozymes are ***,activity prediction and rational design of nanozymes are focused by highlighting the methods of density functional theory,machine learning,biomimetic and chemical ***,synergistic theranostic strategy of nanozymes are ***,current challenges and future prospects of nanozymes used for tumor theranostic are outlined,including selectivity,biosafety,repeatability and stability,in-depth catalytic mechanism,predicting and evaluating activities.

关键词： Nanozymes Classification Prediction and design catalytic mechanism Tumor theranostics

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