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Coupled intramolecular/heterointerfacial electron transfer in polyelectrolyte-shielded Iso-type black phosphorus hetero-structure boosts oxygen reduction kinetics

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Journal of Energy chemistry 2021年第12期30卷 468-476,I0011页

作者： Zhongke Yuan Jing Li Zhengsong Fang Meijia Yang Kancheng Mai Dingshan Yu key laboratory for Polymeric Composite and Functional Materials of Ministry of Education Key Laboratory of High Performance Polymer-based Composites of Guangdong ProvinceSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275GuangdongChina

Searching new structured black phosphorus(BP)and exploring intriguing functions and applications have become a hot topic so ***,we introduce a novel Iso-type black phosphorus heterostructure guided by first principle calculation,which features unique heterointerface and electronic coupling interaction via stacking assembly of exfoliated black phosphorus(EBP)and amine-functionalized EBP(N-EBP).Inspired by the theoretical results,we constructed the Iso-type heterostructure comprising of ultrathin exfoliated few-layered EBP and N-EBP,both of which were derived from identical bulk *** purposive amine-functionalization not only creates positively-charged P atoms on N-EBP as effective active sites via N-induced intramolecular electron transfer(IET)but also endows N-EBP with lower work function relative to EBP,while the unique EBP/N-EBP Iso-type heterostructure engenders directional heterointerfacial electron transfer(HET).The coupled IET/HET effects optimize the charge redistribution to afford favorable O_(2)*** this case,our unique strategy for the first time exploits the inherent catalytic capability of BP toward the oxygen reduction reaction(ORR)and enables the first use of BP as metal-free ORR catalysts for Zn-air *** newly-designed heterostructure facilitates a 4-e^(-)transfer ORR relative to inactive EBP or ***,the polymer-shielded heterostructure acts as efficient air electrodes to endow a primary Zn-air cell with high stability,large capacity and high energy density—superior to the commercial Pt/C-enabled *** study as the first report on metal-free BP-based ORR catalysts and air electrodes not only extends BP's application scopes but also renders new insight toward design of electronically-coupled superstructures for energy-related applications.

关键词： Black phosphorus Iso-type heterostructure Intramolecular electron transfer Heterointerfacial electron transfer Oxygen reduction

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Carbon-Involved Near-Surface Evolution of Cobalt Nanocatalysts:An in Situ Study

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CCS chemistry 2021年第11期3卷 154-167页

作者： Feng Yang Haofei Zhao Wu Wang Qidong Liu Xu Liu Yuecong Hu Xinrui Zhang Sheng Zhu Dongsheng He Yingying Xu Jiaqing He Rongming Wang Yan Li Beijing National laboratory for Molecular Science Key Laboratory for the Physics and Chemistry of NanodevicesState Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 department of chemistry Guangdong Provincial Key Laboratory of Catalytic ChemistrySouthern University of Science and TechnologyShenzhenGuangdong 518055 Beijing Advanced Innovation Center for Materials Genome Engineering Center for Green InnovationBeijing Key Laboratory for Magneto-Photoelectrical Composite and Interface ScienceSchool of Mathematics and PhysicsUniversity of Science and Technology BeijingBeijing 100083 department of Physics Southern University of Science and TechnologyShenzhenGuangdong 518055 Core Research Facilities Southern University of Science and TechnologyShenzhenGuangdong 518055

When carbon-containing species are involved in reactions catalyzed by transition metals at high temperature,the diffusion of carbon on or in catalysts dramatically influences the catalytic *** information on the carbon-diffusioninvolved evolution of catalysts at the atomic level is crucial for understanding the reaction mechanism yet also *** the chemical vapor deposition process of single-walled carbon nanotubes(SWCNTs),we recorded in situ the catalyst state(solid and molten)composition as well as near-surface structural and chemical evolution at the cobalt catalyst-tube interface with carbon permeation using aberration-corrected environmental transmission electron microscopy and synchrotron X-ray absorption *** nucleation of SWCNTs was linked with an alternating dissolving and precipitating cycle of carbon in catalysts close to the nucleation *** the dynamics of carbon atoms in catalysts brings deeper insight into the growth mechanism of SWCNTs and facilitates inferring mechanisms of other *** methodologies developed here will find broad applications in studying catalytic and other processes.

关键词： carbon nanotube catalysts chemical vapor deposition structure evolution aberrationcorrected environmental transmission electron microscopy

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Facet-selective growth of MOF-on-MOF heterostructures enables etching-free synthesis of highly-open Co/N-doped carbon nanoframes for efficient catalysis

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Science China chemistry 2022年第12期65卷 2450-2461页

作者： Yaohui Wu Liyu Chen Xianfeng Yang Yingwei Li Kui Shen guangdong provincial key laboratory of Fuel Cell Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou510640China State key laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou510640China Analytical and Testing Centre South China University of TechnologyGuangzhou510640China

Highly-open nanoframe structures consisting of interconnected and exposed ridges are highly desirable for achieving efficient catalysis,but preparing them by a facile etching-free methodology is still a very daunting ***,we propose a novel metal-organic framework(MOF)-assisted and etching-free strategy for the construction of Co/N-doped carbon nanoframes with highly-open and precisely-controllable *** strategy is based on the face-selective epitaxial growth of ZIF-67 on the 36{110}facets of 72-facet ZIF-8 to form an unprecedented anisotropic ZIF-67-on-ZIF-8 heterostructure,which is subsequently pyrolyzed under Ar atmosphere to realize a solid-to-frame *** highly-open nanoframe structure enables the substrates to readily penetrate into the catalyst interior and thereby create additional exposed active sites,which together with the good mass transport,high atomic utilization and increased surface area are responsible for its remarkably enhanced catalytic activity for the biomass valorisation when compared with its solid and closed hollow *** study could shed valuable insights into the design and preparation of various highly-open nanoframes with abundant exposed active species by using an etching-free strategy for efficient catalysis and beyond.

关键词： metal-organic frameworks etching-free synthesis highly-open nanoframes pyrolysis efficient catalysis

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Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support

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Energy & Environmental Materials 2024年第5期7卷 272-282页

作者： Shamraiz Hussain Talib Beenish Bashir Muhammad Ajmal Khan Babar Ali Sharmarke Mohamed Ahsanulhaq Qurashi Jun Li Advanced Materials chemistry Center(AMCC) Khalifa University of Science and TechnologyAbu Dhabi P.O.Box 127788UAE department of chemistry Khalifa University of Science and TechnologyAbu Dhabi P.O.Box 127788UAE department of chemistry and Biochemistry George Mason University4400 University DriveFairfaxVirginia 22030USA Interdisciplinary Research Center for Refining and Advanced Chemicals King Fahd University of Petroleum&MineralsDhahran 31261Saudi Arabia department of chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education Tsinghua UniversityBeijing 100084China department of chemistry and guangdong provincial key laboratory of catalytic chemistry Southern University of Science and TechnologyShenzhen 518055China

Single-atom catalysts(SACs)have received significant interest for optimizing metal atom utilization and superior catalytic performance in hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and oxygen reduction reaction(ORR).In this study,we investigate a range of single-transition metal(STM_(1)=Sc_(1),Ti_(1),V_(1),Cr_(1),Mn_(1),Fe_(1),Co_(1),Ni_(1),Cu_(1),Zr_(1),Nb_(1),Mo_(1),Ru_(1),Rh_(1),Pd_(1),Ag_(1),W_(1),Re_(1),Os_(1),Ir_(1),Pt_(1),and Au_(1))atoms supported on graphyne(GY)surface for HER/OER and ORR using first-principle *** initio molecular dynamics(AIMD)simulations and phonon dispersion spectra reveal the dynamic and thermal stabilities of the GY *** exceptional stability of all supported STM_(1)atoms within the H1 cavity of the GY surface exists in an isolated form,facilitating the uniform distribution and proper arrangement of single atoms on *** particular,Sc_(1),Co_(1),Fe_(1),and Au_(1)/GY demonstrate promising catalytic efficiency in the HER due to idealisticΔG_(H^(*))values via the Volmer-Heyrovsky ***,Sc_(1)and Au_(1)/GY exhibit superior HER catalytic activity compared to other studied ***_(1)/GY catalyst exhibits higher selectivity and activity for the OER,with an overpotential(0.46 V)comparable to MoC_(2),IrO_(2),and RuO_(2).Also,Rh_(1)and Co_(1)/GY SACs exhibited promising electrocatalysts for the ORR,with an overpotential of 0.36 and0.46 V,***,Co_(1)/GY is a versatile electrocatalyst for metal-air batteries and *** study further incorporates computational analysis of the kinetic potential energy barriers of Co_(1)and Rh_(1)in the OER and ORR.A strong correlation is found between the estimated kinetic activation barriers for the thermodynamic outcomes and all proton-coupled electron transfer *** establish a relation for the Gibbs free energy of intermediates to understand the mechanism of SACs supported on STM,/GY and introduce a key *** stu

关键词： Oxygen Reduction Reaction Graphyne Support Hydrogen Evolution Reaction Oxygen Evolution Reaction Single-Atom Catalyst Water Splitting

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Pitfalls of restriction enzyme analysis in identifying, characterizing,typing, and naming viral pathogens in the era of whole genome data, as illustrated by HAdV type 55

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Virologica Sinica 2016年第5期31卷 448-453页

作者： Qiwei Zhang Shoaleh Dehghan Donald Seto Biosafety Level-3 laboratory School of Public HealthSouthern Medical University(Guangdong Provincial Key Laboratory of Tropical Disease Research) chemistry department American University Bioinformatics and Computational Biology Program School of Systems BiologyGeorge Mason University

Restriction endonuclease analysis(REA),or restriction fragment length polymorphism(RFLP),was useful for identifying and determining the relatedness and putative identities of microbial strains(Tang et al.,1997)and for... 详细信息

关键词： and naming viral pathogens in the era of whole genome data DLL QS characterizing,typing Pitfalls of restriction enzyme analysis in identifying REA type

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A Ruddlesden-Popper oxide as a carbon dioxide tolerant cathode for solid oxide fuel cells that operate at intermediate temperatures

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Chinese Journal of Chemical Engineering 2023年第4期56卷 25-32页

作者： Shujun Peng Song Lei Sisi Wen Jian Xue Haihui Wang School of chemistry&Chemical Engineering Jinggangshan UniversityJi'an 343009China School of chemistry&Chemical Engineering Guangdong Provincial Key Lab of Green Chemical Product TechnologySouth China University of TechnologyGuangzhou 510640China Beijing key laboratory of Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Solid oxide fuel cells(SOFCs) that operate at intermediate temperatures of 600 to 800℃ have recently received increased attention due to their improved durability, more rapid startup and shutdown, better sealing and lower cost than their counterparts operate at high temperatures. Nevertheless, intermediatetemperature SOFCs(IT-SOFCs) with popular perovskite cathodes contain alkaline-earth elements, which are prone to reaction with carbon dioxide(CO_(2)), even when the CO_(2) content is comparatively low. In this work, an alkaline-earth metal-free Ruddlesden-Popper oxide, Nd_(1.8)La_(0.2)Ni_(0.74)Cu_(0.21)Ga_(0.05)O_(4+δ)(NLNCG), is developed for IT-SOFC cathodes. The cell is based on an electrolyte with 8%(mol) Y_(2)O_(3)-stabilized Zr O_(2)(8YSZ). The NLNCG cathode exhibits an excellent CO_(2) tolerance, as proven by thermogravimetry analysis,in situ X-ray diffraction, I-V-P test, and electrochemical impedance spectroscopy(EIS), and stability measurements. The anode-supported single-cell Ni O-YSZ|YSZ|NLNCG outputs a peak power density of 0.522 W·cm^(-2) at 800℃. These findings suggest that NLNCG could be a highly suitable cathode material with CO_(2) tolerance for IT-SOFCs.

关键词： Fuel cell Hydrogen Kinetics Catalyst CO_(2)tolerance

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Direct synthesis of ordered mesoporous ZSM-5 zeolites from in situ crystallization of carbonaceous SBA-15

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Science China chemistry 2017年第12期60卷 1588-1595页

作者： Fangfang Wei Qiuyun Zhang Hong Wu Changyan Cao Weiguo Song School of chemistry and Chemical Engineering Anshun UniversityAnshun 561000China key laboratory of Functional Materials and Resource chemistry of Guizhou provincial Education department Anshun UniversityAnshun 561000China College of chemistry and Material Engineering Liupanshui Normal UniversityLiupanshui 553004China Beijing National laboratory of Molecular Sciences Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Two types of ordered mesoporous ZSM-5 zeolites with different mesopores were synthesized by a two-step method. First, carbonaceous SBA- 15 was produced by in situ carbonization of SBA- 15/P 123 composite. Then the obtained SBA- 15/C composite was transformed into crystallized mesoporous ZSM-5 by impregnation TPAOH followed by steam-assisted crystallization. The final calcined samples synthesized with typical SBA-15/P 123 precursor showed a wormlike morphology with the mean mesopore size of 4.6 nm, while samples synthesized with the addition of trimethylbenzene as swelling agent in the precursor exhibited the morphology of microsphere with the mesopore size of about 9.5 nm. Both two types of mesoporous ZSM-5 zeolites exhibited large surface area and mesopore structure. The steam-assisted crystallization （SAC） was performed with lower consumption of solvents. This two-step method may also be suitable for synthesizing other ordered mesoporous zeolites used as catalysts in some catatytic processes.

关键词： mesoporous zeolites ZSM-5 in situ carbonization steam-assistant crystallization

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Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

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Chinese Journal of Chemical Engineering 2024年第7期71卷 172-182页

作者： Runnong Yang Wuyuan Liu Zhaoying Wang Ming Sun Guangying Fu Zihan Gao Wenjian Jiao Rui Li Lin Yu guangdong provincial laboratory of chemistry and Fine Chemical Engineering Jieyang Center Jieyang 515200China guangdong Engineering Technology Research Center of Modern Fine Chemical Engineering School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006China key laboratory of Bioinorganic and Synthetic chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Testing and Certification Business department China Automotive Technology and Research Center Company LimitedWuhan 430056China guangdong Foran Technology Company Limited Foshan 528000China

The Cu-exchanged SSZ-13 with the small-pore chabazite framework is considered as a highly efficient catalyst for selective catalytic reduction of NO with NH_(3)(NH_(3)-SCR).In order to further improve the catalytic property,a series of Mn ion-assisted Cu/SSZ-13 powder catalysts were prepared by co-exchange method and stepwise exchange *** is found that the NH_(3)-SCR activity,N_(2) selectivity,hydrothermal stability and sulfur resistance of Cu/SSZ-13 are promoted by introducing a minority of Mn(0.15%to 0.23%(mass))through co-exchange *** results reveal that the Cu,Mn co-exchange enables the higher amounts of Cu^(2+)active sites,the abundant medium strong and strong acid,the optimized ratio of Lewis acid to Brønsted acid etc.,which are required for a good NH_(3)-SCR catalytic property over broad temperature range and under harsh working ***,a monolithic catalyst was prepared by impregnating a cordierite ceramic support into the coating slurry containing the optimized CuMn/SSZ-13 *** diesel engine bench tests show that Cu,Mn co-exchange gives the monolith catalyst a better catalytic property than commercial *** work provides an important guidance for the rational design of secondary-ion-assisted zeolites applied in NH_(3)-SCR.

关键词： MnCu/SSZ-13 Co-exchange Zeolite Catalysis Selective catalytic reduction

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Boosting fire safety and mechanical performance of thermoplastic polyurethane by the face-to-face two-dimensional phosphorene/MXene architecture

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Journal of Materials Science & Technology 2022年第34期129卷 27-39页

作者： Yong Luo Yuhui Xie Wei Geng Junhan Chu Hua Wu Delong Xie Xinxin Sheng Yi Mei Yunnan provincial key laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials The Higher Educational Key Laboratory for Phosphorus Chemical Engineering of Yunnan ProvinceFaculty of Chemical EngineeringKunming University of Science and TechnologyKunming 650500China guangdong provincial key laboratory of Functional Soft Condensed Matter School of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006China department of chemistry and Applied Biosciences Institute for Chemical and BioengineeringETH ZurichZurich 8093Switzerland

Black phosphorus(BP), as one of the most promising fillers for flame retarding polymer, has been seriously limited in practical application, due to the agglomeration and poor structural stability ***, the BP was modified by MXene and polydopamine(PDA) via ultrasonication and dopamine modification strategy to improve the structural stability and dispersibility in the matrix. Then, the obtained(BP-MXene@PDA) nanohybrid was employed to promote the mechanical performance, thermal stability,and flame retardancy of thermoplastic polyurethane elastomer(TPU). The resultant TPU composite containing 2 wt.% of BP1-MXene2@PDA showed a 19.2% improvement in the tensile strength and a 13.8%increase in the elongation at break compared to those of the pure TPU. The thermogravimetric analysis suggested that BP-MXene@PDA clearly enhances the thermal stability of TPU composites. Furthermore,the introduction of the BP-MXene@PDA nanohybrids could considerably improve the flame retardancy of TPU composite, i.e., 64.2% and 27.3% decrease in peak heat release rate and total heat release, respectively. The flame-retardant mechanisms of TPU/BP-MXene@PDA in the gas phase and condensed phase were investigated systematically. This work provides a novel strategy to simultaneously enhance the fire safety and mechanical properties of TPU, thus expanding its industrial applications.

关键词： Thermoplastic polyurethane elastomer Black phosphorus MXene Mechanical properties Flame retardancy

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Metal-Organic Framework Nanozyme Enabling Dual-Functional Photo-lnduced Charge Transfer and Biomimetic Precipitation for Advanced Organic Photoelectrochemical Transistor Bioanalysis

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Chinese Journal of chemistry 2024年第17期42卷 1999-2004页

作者： Ke-Xin Xu Cheng Yuan Hao Lou Feng-Zao Chen Ling Zhang Guangxu Chen De-Man Han Wei-Wei Zhao state key laboratory of Analytical chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjingJiangsu210023China School of Pharmaceutical and Chemical Engineering Taizhou UniversityTaizhouJjiangsu 318000China School of Environment and Energy State Key Laboratory of Luminescent Materials and DevicesGuangdong Provincial Key Laboratory of Atmospheric Environment and Pollution ControlSouth China University of TechnologyGuangzhouGuangdong 510006China

We report herein the first observation of MoF nanozyme enabling dual-functional photo-induced charge transfer and biomimetic precipitation for advanced organic photoelectrochemical transistor(OPECT)***,Fe/Co-MIL-88,serving simultaneously as the semiconductor and nanozyme,was explored as a dual-functional gating module in *** light llumination,it could accelerate the charge transfer of the photogate to produce enhanced photo-induced ***,its catalytic property could efficiently produce biomimetic precipitation to block the nanopores in Fe/Co-MIL-88 and thus alter the device characteristics.

关键词： Metal-organic frameworks Nanozymes Organic transistor Photoelectrochemical Biosensing Electrodes

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