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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 viable.Cobalt phosphide(Co-P)has emerged as a catalyst of high potential owing to its high catalytic activity and durability in water splitting.This paper systematically reviews the latest advances in the development of Co-P-based materials for use in water splitting.The essential effects of P in enhancing the catalytic performance of the hydrogen evolution reaction and oxygen evolution reaction are first outlined.Then,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 experiment.Along with these optimization strategies,the understanding of the inherent mechanism of enhanced catalytic performance is also discussed.Finally,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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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 application.In this study,a novel Ni-Nb/rGO nanocomposite catalyst was successfully prepared by one-spot hydrothermal and sub-sequent calcination methods.The novel Ni-Nb/rGO nanocomposite exhibits an exceptional catalytic effect on improving MgH_(2) sorption properties.Specifically,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℃,respectively.Furthermore,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 temperatures.Additionally,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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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 production.Recently,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 effects.Thus,various nanozymes have been developed and used for tumor therapy.In this review,more than 270 research articles are discussed systematically to present progress in the past five years.First,the discovery and development of nanozymes are summarized.Second,classification and catalytic mechanism of nanozymes are discussed.Third,activity prediction and rational design of nanozymes are focused by highlighting the methods of density functional theory,machine learning,biomimetic and chemical design.Then,synergistic theranostic strategy of nanozymes are introduced.Finally,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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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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Activation of hydrogen peroxide by molybdenum disulfide as Fenton-like catalyst and cocatalyst:Phase-dependent catalytic performance and degradation mechanism

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Chinese Chemical Letters 2023年第5期34卷 403-407页

作者： Yue Li Bo Yu Huimin Li Bo Liu Xiang Yu Kewei Zhang Gang Qin Jiahao Lu Lihui Zhang Longlu Wang School of Chemical and Printing-Dyeing Engineering Henan International Joint Laboratory of Rare Earth Composite MaterialsHenan University of EngineeringXinzheng 451191China School of Material Science and Engineering Henan Polytechnic UniversityJiaozuo 454001China College of Electronic and Optical Engineering&College of Microelectronics Institute of Flexible Electronics(Future Technology)Nanjing University of Posts&TelecommunicationsNanjing 210023China

Molybdenum disulfide(Mo S_(2))has attracted great attention in hydrogen peroxide(H_(2)O_(2))activation as a Fenton-like catalyst and cocatalyst,but the distinct mechanism of generating^(·)OH remains unclear.In this paper,the metallic 1T phase and semiconducting 2H phase of Mo S_(2)nanosheets were prepared and applied in MoS_(2)/H_(2)O_(2)and MoS_(2)/Fe^(2+)/H_(2)O_(2)systems with and without light irradiation.Compared with2H-MoS_(2),1T-MoS_(2)exhibited superior removal rates in degrading organic pollutants in the two systems under light irradiation.However,the phase had little effect on activating H_(2)O_(2)in the Mo S_(2)/H_(2)O_(2)system under dark conditions.This is because it was difficult for the surface^(·)OH_(ads)generated in the Mo S_(2)/H_(2)O_(2)system to diffuse into solution,while the^(·)OH_(free)radicals were mainly responsible for degrading organic pollutants.When introducing light irradiation,external energy may accelerate the desorption of^(·)OH_(ads)into^(·)OH_(free.)Interestingly,the conversion between Mo^(4+)and Mo^(5+)triggered the decomposition of H_(2)O_(2)in the Fenton-like reaction,while the cycle of Mo^(4+)/Mo^(6+)promoted the regeneration of Fe^(3+)when employing 1T-MoS_(2)as a cocatalyst.Meanwhile,the 1T-MoS_(2)catalysts exhibited excellent stability and ability to degrade various organics in the two systems.This work offers deeper insight into the Mo S_(2)-based Fenton-like and cocatalytic mechanisms.

关键词： Molybdenum sulfate Phase Fenton-like catalyst Cocatalyst catalytic mechanism

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Highly efficient catalyst for 1,1,2-trichloroethane dehydrochlorination via BN_(3) frustrated Lewis acid-base pairs

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Nano Research 2024年第6期17卷 4773-4781页

作者： Yuxue Yue Fangmin Zuo Bolin Wang Xiaoling Xian Jun Tang Haifeng Zhang Zilong Zhang Qingping Ke Wei Chen School of Chemical Engineering Northeast Electric Power UniversityJilin 132012China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014China Key Laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China College of Chemistry and Chemical Engineering Anhui University of TechnologyMaanshan 243002China

In this study,a novel non-metallic carbon-based catalyst co-doped with boron and nitrogen(B,N)was successfully synthesized.By precisely controlling the carbonization temperature of a binary mixed ionic liquid,we selectively modified the doping site structure,ultimately constructing a B,N co-doped frustrated Lewis acid-base pair catalyst.This catalyst exhibited remarkable catalytic activity,selectivity,and stability in the dehydrochlorination reaction of 1,1,2-trichloroethane(TCE).Detailed characterization and theoretical calculations revealed that the primary active center of this catalyst was the BN_(3)configuration.Compared to conventional graphitic N structures,the BN_(3)structure had a higher p-band center,ensuring superior adsorption and activation capabilities for TCE during the reaction.Within the BN_(3)site,three negatively charged nitrogen atoms acted as Lewis bases,while positively charged boron atoms acted as Lewis acids.This synergistic interaction facilitated the specific dissociation of chlorine and hydrogen atoms from TCE,significantly enhancing the 1,1-dichloroethene selectivity.Through this research,we not only explored the active site structure and catalytic mechanism of B,N co-doped catalysts in depth but also provided an efficient,selective,and stable catalyst for the dehydrochlorination of TCE,contributing significantly to the development of non-metallic catalysts.

关键词： B N co-doped sites dehydrochlorination frustrated Lewis acid-base pairs catalytic mechanism

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Deciphering the high-carbonization-temperature triggered enzymatic activity of wool-derived N,S-co-doped carbon nanosheets

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Chinese Chemical Letters 2024年第3期35卷 182-188页

作者： Jiachen Zhao Deshuai Yu Jianmin Chen Shihao Lin Yonghua Tang Chaoyu Fan Dongfang Zhou Youhui Lin Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchXiamen UniversityXiamen 361005China School of Pharmacy and Medical Technology Putian UniversityPutian 351100China Key Laboratory of Mental Health of the Ministry of Education NMPA Key Laboratory for Research and Evaluation of Drug Metabolism&Guangdong Provincial Key Laboratory of New Drug ScreeningSchool of Pharmaceutical SciencesSouthern Medical UniversityGuangzhou 510515China Key Laboratory of Pharmaceutical Analysis and Laboratory Medicine(Putian University) Fujian Province UniversityPutian 351100China

It is well-established that high carbonization temperature will trigger the enzyme-like activity of carbon-based materials.However,the catalytic mechanism is still ambiguous,which hinders the further rational design of nanomaterials as enzyme mimics.Hereby,N,S-rich carbonized wool nanosheets(CWs)were synthesized at different pyrolysis temperatures.As expected,only CWs treated with high-temperature possess intrinsic oxidase-and peroxidase-like activities.Meanwhile,density functional theory(DFT)calculations demonstrate that graphitic nitrogen and the co-existence of nitrogen and sulfur in the carbon matrix serve as the active sites for the enzyme-like process.More importantly,combining theoretical calculations and experimental observations,the high-temperature triggered catalytic mechanism can be ascribed to the fact that an appropriate high-temperature maximizes the graphitization degree to a certain extent,at which most of the catalytic active sites are well retained rather than evaporating.Moreover,coupling with excellent photothermal conversion efficiency and catalytic performance,CWs can be applied to photothermal-catalytic cancer therapy under near-infrared region(NIR)light irradiation.We believe this work will contribute to understanding the catalytic mechanism of carbon-based nanozymes and promote the development of new biomedical and pharmaceutical applications.

关键词： Carbon-based nanozyme catalytic mechanism Density functional theory High-temperature carbonization

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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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缺陷钴氧化物中选择性锚定Pd单原子用于高效锂氧电池

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Science China Materials 2024年第5期67卷 1433-1444页

作者：郑健张文静李泰广陈步天柳冲张天然刘向峰 Center of Materials Science and Optoelectronics Engineering College of Materials Science and Optoelectronic TechnologyUniversity of Chinese Academy of SciencesBeijing100049China

非质子锂氧电池基于锂金属与氧的可逆反应生成Li_(2)O_(2),可提供极高的理论能量密度.然而,Li_(2)O_(2)的成核/消除机制仍然不清楚.因此,构建能在原子水平上深入了解催化机理的催化剂体系,是开发高性能锂氧电池的关键.在此,我们报道了... 详细信息

非质子锂氧电池基于锂金属与氧的可逆反应生成Li_(2)O_(2),可提供极高的理论能量密度.然而,Li_(2)O_(2)的成核/消除机制仍然不清楚.因此,构建能在原子水平上深入了解催化机理的催化剂体系,是开发高性能锂氧电池的关键.在此,我们报道了一种在富氧空位的Co_(3)O_(4)(Pd1-Co_(3)O_(4x))中实现Pd单原子选择性锚定的策略.原子水平表征技术揭示了Pd原子优先地结合到缺陷Co_(3)O_(4)的四面体位点.理论计算表明,选择性锚定的Pd单原子与氧空位的耦合引起了明显的电荷重分布,这可以有效地提高Pd 4d轨道在费米能级附近的能带占用率,促进电子转移,有利于中间体的吸附.这种双重相互作用不仅可以调节放电过程中Li_(2)O_(2)的成核生长过程,而且有利于Li_(2)O_(2)上的电子云的离域,减弱Li-O键的强度,从而促进Li_(2)O_(2)在充电过程中的分解.本研究对锂氧电池在原子水平上的催化机理和高效催化剂的合理设计提出了一些见解.

关键词： Pt single-atom catalyst tetrahedral sites oxygen vacancies catalytic mechanism Li-O_(2)batteries

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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 clear.In 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 1-dodecene.The 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 1-dodecene.The 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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