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Fe-N_(x) sites coupled with core-shell FeS@C nanoparticles to boost the oxygen catalysis for rechargeable Zn-air batteries

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Journal of Energy Chemistry 2024年第3期90卷 565-577,I0013页

作者： katam srinivas Zhuo Chen Anran Chen Fei Ma Ming-qiang Zhu Yuanfu Chen School of Integrated Circuit Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengdu 610054SichuanChina College of Mechanical and Electronic Engineering Northwest A&F UniversityYangling 712100ShaanxiChina School of Materials and Energy Yunnan UniversityKunming 650091YunnanChina

The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic ***,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent *** to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling ***,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based *** work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.

关键词： Fe-N_(x)sites Core-shell FeS@C Synergistic interactions Oxygen reduction reaction Zn-air battery

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Controlling the solid-state luminescence of gold(I) N-heterocyclic carbene complexes through changes in the structure of molecular aggregates

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Science China Chemistry 2018年第8期61卷 957-965页

作者： Arruri Sathyanarayana Shin-ya Nakamura Kyohei Hisano Osamu Tsutsumi katam srinivas Ganesan Prabusankar Department of Applied Chemistry Ritsumeikan University 1-1-1 Nojihigashi Department of Chemistry Indian Institute of Technology

Thermally stable, solid-state luminescent organic materials are highly desired for the development of practical *** we synthesized new gold(I) complexes with N-heterocyclic carbene ligands, which have the ability to form strong metalorganic bond. Consequently, their thermochemical stability is enhanced at temperatures around 300 °C. Precise design of the molecular structure of the ligands, with a focus on ensuring low steric hindrance around Au atoms in order to limit disturbances to Au/Au interactions, provided a complex with a densely packed crystal with a shorter intermolecular Au–Au distance(3.17 ?)than the typical distance. In the solid state, this complex exhibited strong aurophilic interactions, which generated intense phosphorescence even in air at room temperature(quantum yield=16%) in spite of absence of any phosphorescence in *** behavior is characteristic for solid-state luminescence referred to as aggregation-controlled emission. Furthermore, the gold(I) complex displays capacity for mechano-and vapo-chromism—that is, the ability to change color reversibly in response to the application of external stimuli. We believe that the proposed design framework, which involves controlling thermal stability and luminescence property separately, provides a new opportunity for the development of practical applications using solid-state luminescent organic molecules.

关键词： Au complex N-heterocyclic carbene phosphorescence mechanochromism aggregation-induced emission

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N-doped CNTs capped with carbon layer armored CoFe alloy as highly stable bifunctional catalyst for oxygen electrocatalysis

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Nano Research 2022年第5期15卷 3971-3979页

作者： Bin Wang katam srinivas Yanfang Liu Dawei Liu Xiaojuan Zhang Wanli Zhang Yuanfu Chen State Key Laboratory of Electronic Thin Films and Integrated Devices University of Electronic Science and Technology of ChinaChengdu 610054China College of Science and Institute of Oxygen SupplyTibet UniversityLhasa 850000China

Designing and fabricating the bifunctional electrocatalysts for the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)has long posed an uphill and pressing task for the interconversion of electricity and *** this in mind,herein,we propose a novel hierarchical nanoarchitecture of N-doped carbon nanotubes capped with carbon layer armored CoFe alloy(CoFe@NC-NT),which is facilely fabricated by spray drying and subsequent annealing *** a bifunctional electrocatalyst,the well-designed CoFe@NC-NT shows a remarkably low overpotential of 257 mV and a half-wave potential of 0.74 V to obtain 10 mA·cm^(-2)in OER and ORR,***,it is also characterized by exceptional operating stability to meet practical application for Zn-air *** high catalytic activity of CoFe@NC-NT is attributed to the tight contact between the highly conductive nanotubes and metal alloy *** the qualified stability is ascribed to the coating effect of carbon layer shell to alloy *** the unique structural evolution with enhanced oxygen-involved reaction activity,we believe that this work can provide an appealing innovative approach towards the directed self-assembly of functional nanostructures to realize satisfying overall performance.

关键词： oxygen electrocatalysis metal alloy coating effect self-assembly Zn-air battery

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Surface modification of metal-organic frameworks under sublimated iron-atmosphere by controlled carbonization for boosted oxygen evolution reaction

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Nano Research 2022年第7期15卷 5884-5894页

作者： katam srinivas Xin Chen Dawei Liu Fei Ma Xiaojuan Zhang Wanli Zhang Hua Lin Yuanfu Chen School of Electronic Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengdu 610054China School of Materials and Energy Southwest UniversityChongqing 400715China College of Science and Institute of Oxygen SupplyTibet UniversityLhasa 850000China

Development of cost-effective,efficient,and durable electrocatalysts for oxygen evolution reaction(OER)with fast kinetic reaction is highly significant,considering the elevated thermodynamic energy barrier involved in water *** overcome such challenges,an innovative vapor phased iron-doping strategy is employed on carbon nanotubes(CNT)-interlinked metalorganic framework(MOF)nanosheets(Ni-MOF@CNT)to obtain mixed metal oxide and metal heteronanoparticles superficially implanted partially(semi)-decomposed MOF nanosheets(Ni-M@C-400).These semi-MOF nanosheets attain the structural privileges related to MOF-nanostructure,mixed metal nanoparticles synergism,interconnected-CNT assisted high conductivity,and mechanical *** a result,Ni-M@C-400 exhibits exceptional OER activity with overpotential as low as 229 mV to reach the benchmark current density of 10 mA/cm^(2)(η10)and exhibits greatly reduced thermodynamic barrier(Tafel slopes of 40.51 mV/dec)along with significant durability for~60 *** importantly,this sublimated iron-doped semi-MOF(Ni-M@C-400)displays significantly better OER performance over the corresponding annealed bimetallic MOF(NiFe-M@C-400:270 mV atη10).Moreover,the successful incorporation of vapor phased iron into variety of MOFs(Cr,Mn,Co,Ni,and Cu)approved its uniqueness and the *** work provides an innovative vapor phased heteroatom-doping strategy to develop costeffective and efficient electrocatalysts for water electrolysis.

关键词： metal-organic frameworks(MOFs) semi-MOFs controlled carbonization heteronanoparticles oxygen evolution reaction

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Fe_(2)P nanoparticles embedded on Ni_(2)P nanosheets as highly efficient and stable bifunctional electrocatalysts for water splitting

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Journal of Materials Science & Technology 2022年第10期105卷 266-273页

作者： Xinqiang Wang Bin Wang Yuanfu Chen Mengya Wang Qi Wu katam srinivas Bo Yu Xiaojuan Zhang Fei Ma Wanli Zhang School of Electronic Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengdu 610054China School of Science and Institute of Oxygen SupplyTibet UniversityLhasa 850000China

It is urgent to develop highly efficient,stable and low-cost bifunctional electrocatalysts for overall water ***,an iron-nickel phosphide(Fe_(2)P/Ni_(2)P)heterostructure,constructed by Fe_(2)P nanoparticles embedded on Ni_(2)P nanosheets,is strategically fabricated on nickel foam via a facile *** a bifunctional electrocatalyst,the Fe_(2)P/Ni_(2)P heterostructure delivers a very low overpotential of 64 m V(or 185m V)to reach current density of 10 m A cm^(-2)for hydrogen(or oxygen)evolution *** simultaneously employed as both the anode and cathode electrodes,it demonstrates an ultralow cell voltage of1.49 V@10 m A cm^(-2)for full water splitting with nearly 100%Faradaic efficiency,and superior long-term stability even over 100 *** functional theory calculations manifest that a strong heterointerface interaction could cause electron redistribution near the Fe_(2)P/Ni_(2)P heterointerface and optimize theΔG_(H)*of P sites,thus enhancing catalytic ***,the 3D porous heterostructure is beneft to expose rich active sites and facilitate ion diffusion and gas bubble release,thus promoting the catalytic *** work opens up a new strategical approach for rational design of metal phosphide-based heterostructures as highly efficient and stable bifunctional electrocatalysts for water splitting.

关键词： Heterostructure Nanosheets Electrocatalyst Overall water splitting

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MoP QDs@graphene as highly efficient electrocatalyst for polysulfide conversion in Li-S batteries

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Journal of Materials Science & Technology 2021年第31期90卷 37-44页

作者： Bo Yu Fei Ma Dongjiang Chen katam srinivas Xiaojuan Zhang Xinqiang Wang Bin Wang Wanli Zhang Zegao Wang Weidong He Yuanfu Chen School of Electronic Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengdu 610054PR China School of Physics University of Electronic Science and Technology of ChinaChengdu 611731PR China School of Science and Institute of Oxygen SupplyTibet UniversityLhasa 850000PR China College of Materials Science and Engineering Sichuan UniversityChengdu 610065PR China

The shuttle effect of lithium polysulfides(LiPSs)and sluggish redox conversion significantly hinder practical implementation of lithium-sulfur batteries(LSBs).To overcome these issues,herein,we present MoP quantum dots anchored N,P-doped graphene(MPQ@G)as a multifunctional LSB *** N,P-doped graphene layers serve as a conductive skeleton to support the MoP QDs which can accelerate the electron transfer,physically hinder the polysulfide migration and thus enhance the electrochemical *** importantly,as a polar and conductive catalyst,MoP QDs provide catalytically active sites for the conversion of *** a result,the LSBs with MPQ@G/S cathodes deliver an elevated initial capacity of 1220.2 mAh g~(-1)at 0.2 C and remain 98.9%after rate cycles,signifying its exceptional cycling ***,it displays a large capacity of 681.2 mAh g~(-1)even at a high rate of 1 *** Li-S pouch cell also presents high specific capacities and preeminent cycling stabilities,confirming its great potential for high-rate *** functional theory calculations demonstrate the improved absorptivity and redox conversion reversibility of *** work provides an efficient strategy to improve composite with highly adsorptive and catalytic properties for high-performance Li-S batteries.

关键词： MoP quantum dots Graphene Electrocatalyst Shuttle effect Li-S batteries

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NbN quantum dots anchored hollow carbon nanorods as efficient polysulfide immobilizer and lithium stabilizer for Li-S full batteries

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Journal of Energy Chemistry 2024年第1期88卷 260-271,I0007页

作者： Fei Ma Zhuo Chen katam srinivas Ziheng Zhang Yu Wu Dawei Liu Hesheng Yu Yue Wang Xinsheng Li Ming-qiang Zhu Qi Wu Yuanfu Chen School of Integrated Circuit Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and TechnologyChengdu 610054SichuanChina College of Science and Institute of Oxygen Supply Center of Tibetan Studies(Everest Research Institute)Tibet UniversityLhasa 850000TibetChina College of Mechanical and Electronic Engineering Northwest A&F UniversityXianyang 712100ShaanxiChina

The shuttle effect of lithium polysulfides(LiPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(Li-S)*** simultaneously address such issues,monodispersed Nb N quantum dots anchored on nitrogen-doped hollow carbon nanorods(NbN@NHCR)are elaborately developed as efficient Li PSs immobilizer and Li stabilizer for high-performance Li-S full *** functional theory(DFT)calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble Li PSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect,but also homogenize the distribution of Li+ions and regulate uniform Li deposition for suppressing Li-dendrite *** a result,the assembled Li-S full batteries(NbN@NHCR-S||Nb N@NHCR-Li)deliver excellent long-term cycling stability with a low decay rate of 0.031%per cycle over 1000 cycles at high rate of 2 *** at a high S loading of 5.8 mg cm^(-2)and a low electrolyte/sulfur ratio of 5.2μL mg^(-1),a large areal capacity of 6.2 mA h cm^(-2)can be achieved in Li-S pouch cell at 0.1 *** study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of Li anode.

关键词： Dual-functional host NbN quantum dots Shuttle effect Dendrite-free Li anode Li-S full batteries

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Recent advances in Fe-N-C single-atom site coupled synergistic catalysts for boosting oxygen reduction reaction

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Electron 2024年第1期2卷 1-38页

作者： katam srinivas Jian Zhen Hesheng Yu Dawei Liu Jian Zhen Ou Ming‐qiang Zhu Yuanfu Chen School of Integrated Circuit Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengduSichuanChina College of Mechanical and Electronic Engineering Northwest A&F UniversityYanglingChina School of Engineering RMIT UniversityMelbourneVictoriaAustralia

Metal-air batteries,fuel cells,and electrochemical H_(2)O2 production currently attract substantial consideration in the energy sector owing to their efficiency and ***,their broader use is hindered by the complex oxygen reduction reaction(ORR)that occurs at cathodes and involves intricate electron *** the significant ORR performance of platinum-based catalysts,their high cost,operational limitations,and susceptibility to methanol poisoning hinder broader *** emphasizes the need for efficient nonprecious metal-based ORR electrocatalysts.A promising approach involves utilizing single-atom catalysts(SACs)featuring metal-nitrogen-carbon(M-N-C)coordination *** offer advantages such as optimal utilization of metal atoms,uniform active centers,precisely defined catalytic sites,and robust metal-support ***,the symmetrical electron distribution around the central metal atom of a single-atom site(M-N4)often results in suboptimal ORR *** challenge can be addressed by carefully tailoring the surrounding environment of the active *** review specifically focuses on recent advancements in the Fe-N4 environment within Fe-N-C *** highlights the promising strategy of coupling Fe-N4 sites with metal clusters and/or nanoparticles,which enhances intrinsic *** capitalizing on the interplay between Fe-N4 sites and associated species,overall ORR performance *** review combines findings from experimental studies and density functional theory simulations,covering synthesis strategies for Fe-N-C coupled synergistic catalysts,characterization techniques,and the influence of associated particles on ORR *** offering a comprehensive outlook,the review aims to encourage research into high-efficiency Fe single-atom sites coupled synergistic catalysts for real-world applications in the coming years.

关键词： electrocatalysis oxygen reduction reaction particle@Fe-N-C single-atom catalysts synergistic catalysts

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