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Inside-out dual-doping effects on tubular catalysts:Structural and chemical variation for advanced oxygen reduction performance

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Nano Research 2022年第1期15卷 361-367页

作者： Yang Gao Debin Kong Jiaxu Liang Daliang Han Bin Wang Quan-Hong Yang Linjie Zhi CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300350China University of Chinese Academy of Sciences Beijing 100049China

dual-doping of carbon,especially the combination of nitrogen and a secondary heteroatom,has been demonstrated efficient to optimize the oxygen reduction reaction(ORR)performance.However,the optimum dual-doping is still not clear due to the lack of strong experimental proofs,which rely on a reliable method to prepare carbon materials that can rule out the interference factors and then emphasize only the doping effects.In this work,an inside-out doping method is reported to prepare carbon submicrotubes(CSTs)as a material to study the principles of designing dual-doping catalysts for ORR.The interference factors including the metal impurities and doping gradient in the bulk phase are excluded,and the doping effects including the structural and chemical variation of carbon are studied.P-doping exhibited a higher pore-forming ability to perforate carbon and a lower doping content,but a higher ORR catalytic activity as compared with S-and B-doped N-CSTs,demonstrating the N,P co-doping is more efficient in making carbon-based catalysts for ORR.First-principle calculations reveal that the edge C situated around the oxidized P site nearby a graphitic N atom is the active site that shows the lowest ORR overpotential comparable to Pt-based catalysts.This study suggests that the catalytic activity of dual-heteroatoms-doped carbons not only depends on the intrinsic chemical bonding between heteroatoms and carbon,but also is affected by the structural variation generated by introducing different atoms,which can be extended to the study of other kinds of functionalization of carbon and potential reactions besides ORR.

关键词： dual-doping phosphorus carbon tubes oxygen reduction metal-free catalysts

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Complementary dual-doping of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode enhances ion-diffusion and stability for Li-ion batteries

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Chinese Chemical Letters 2023年第6期34卷 577-582页

作者： Zhihong Wang Huawei Zhu Haifeng Yu Tao Zhang Yanjie Hu Hao Jiang Chunzhong Li Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China Key Laboratory for Ultrafine Materials of Ministry of Education School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Lab of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China

The Ni-richLiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered cathodes endow Li-ion batteries(LIBs)with high energy density.However,they usually suffer from limited ion-diffusion and structural instability during cycling.Although doping strategy can effectively alleviate these issues,the coupling effects of multi-element doping and the corresponding performance enhancement mechanism have been yet unclear.Here,we report a Zr/Ti dual-doped NCM811 cathode material(ZT-NCM811),in which Zr-ion is doped into both transition metal(TM)layers and lithium layers and Ti-ion is only distributed in TM layers.The dual-doping can effectively enhance crystal structure stability via inhibiting the lattice collapse along c-axis and decreasing the Li/Ni disorder.Meantime,the lattice oxygen escape is also greatly reduced due to the presence of stronger Zr-O and Ti-O bonds,further mitigating the crystal surface parasitic reactions with electrolyte.The resultant ZT-NCM811 exhibits high specific capacity of 124 m Ah/g at even 10 C,much higher than undoped and single-doped NCM811,and a retention of 98.8%at 1 C after 100 cycles.The assembled ZT-NCM811/graphite full cell also delivers superior battery performances and durability.

关键词： LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) dual-doping High power Cycling stability Li-ion batteries

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Realizing high thermoelectric performance via selective resonant doping in oxyselenide BiCuSeO

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Nano Research 2023年第1期16卷 1679-1687页

作者： Yue-Xing Chen Wenning Qin Adil Mansoor Adeel Abbas Fu Li Guang-xing Liang Ping Fan Muhammad Usman Muzaffar Bushra Jabar Zhen-hua Ge Zhuang-hao Zheng F1 Shenzhen Key Laboratory of Advanced Thin Films and Applications Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong ProvinceCollege of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China Faculty of Materials and Manufacturing Beijing University of TechnologyBeijing 100124China International Center for Quantum Design of Functional Materials(ICQD) Hefei National Laboratory for Physical Sciences at Microscale(HFNL)and CAS Center for Excellence in Quantum Information and Quantum PhysicsUniversity of Science and Technology of ChinaHefei 230026China Faculty of Materials Science and Engineering Kunming University of Science and TechnologyKunming 650093China

Tuning the charge carrier concentration is imperative to optimize the thermoelectric(TE)performance of a material.For BiCuSeO based oxyselenides,doping efforts have been limited to optimizing the carrier concentration.In the present work,dual-doping of In and Pb at Bi site is introduced for p-type BiCuSeO to realize the electric transport channels with intricate band characteristics to improve the power factor(PF).Herein,the impurity resonant state is realized via doping of resonant dopant In over Pb,where Pb comes forward to optimize the Fermi energy in the dual-doped BiCuSeO system to divulge the significance of complex electronic structure.The manifold roles of dual-doping are used to adjust the elevation of the PF due to the significant enhancement in electrical properties.Thus,the combined experimental and theoretical study shows that the In/Pb dual doping at Bi sites gently reduces bandgap,introduces resonant doping states with shifting down the Fermi level into valence band(VB)with a larger density of state,and thus causes to increase the carrier concentration and effective mass(m*),which are favorable to enhance the electronic transport significantly.As a result,both improved ZTmax=0.87(at 873 K)and high ZTave=0.5(at 300–873 K)are realized for InyBi(1−x)−yPbxCuSeO(where x=0.06 and y=0.04)system.The obtained results successfully demonstrate the effectiveness of the selective dual doping with resonant dopant inducing band manipulation and carrier engineering that can unlock new prospects to develop high TE materials.

关键词： thermoelectric material BiCuSeO dual-doping power factor figure of merit

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Al, Zr dual-doped cobalt-free nickel-rich cathode materials for lithium-ion batteries

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Progress in Natural Science:Materials International 2023年第1期33卷 108-115页

作者： Xinxin Tan Wenjie Peng Meng Wang Gui Luo Zhixing Wang Guochun Yan Huajun Guo Qihou Li Jiexi Wang School of Metallurgy and Environment Central South University BASF ShanShan Battery Materials Co. LTD Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South University Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy Central South University

Nickel-rich and cobalt-free cathode materials have obvious advantages in the aspects of energy density and economic efficiency. However, these materials are restricted from being used in commercial lithium-ion batteries due to the problems of poor structural stability and rate capability. In this study, the aluminum and zirconium dual-doped Co-free Ni-rich LiNi0.96Mn0.04O2cathode material(NMAZ) is prepared by a facile high-temperature solid-phase method. The obtained NMAZ shows low cation disordering degree owing to the stability of transition metal slabs induced by strong Al–O and Zr–O bonds. Besides, the kinetics of lithium-ion diffusion is significantly improved by larger c-axis and the fast lithium-ion conducting Li2ZrO3layer on the interface. As a result, NMAZ shows an improved capacity retention of 70.3% at 1C after 100 cycles under an elevated temperature(45°C), compared with 50.5% of pure LiNi0.96Mn0.04O2. In addition, it exhibits splendid rate performance even at higher C-rate and better thermal stability compared to bare LiNi0.96Mn0.04O2. Hence, the Al, Zr dualdoped modification is beneficial to improving the structural stability and electrochemical performance of the Ni-rich and Co-free layered oxide cathodes for Li-ion batteries.

关键词： Lithium-ion batteries Ni-rich Co-free Layered oxide cathode dual-doping

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Pulse-potential electrochemistry to boost real-life application of pseudocapacitive dual-doped polypyrrole

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SmartMat 2022年第4期3卷 644-656页

作者： Fang-Fang Sun Wen-Han Li Zi-Hang Huang Wenping Sun Yuhai Dou Ding Yuan Baohua Jia Tianyi Ma Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials Institute of Clean Energy ChemistryCollege of ChemistryLiaoning UniversityShenyangChina School of Science RMIT UniversityMelbourneVictoriaAustralia School of Materials Science and Engineering State Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhouChina Shandong Institute of Advanced Technology JinanChina Institute for Superconducting&Electronic Materials University of WollongongWollongongAustralia

Polypyrrole(PPy)is a very promising pseudocapacitive electrode material for supercapacitors.However,the poor electrochemical performances and cycling stability caused by volumetric change and counterion drain severely limited its practical application and commercialization.Herein,we present a pulsepotential polymerization strategy for uniformly depositing a dual-doped PPy with ordered and shorter molecular structure by balancing the concentration polarization.Such a strategy ensures more homogeneous stress distribution of PPy during ultralong cycling tests and improves the cycle stability.Moreover,the pulse-potential polymerized PPy with dual anion doping behavior induces enhanced protonation level and improved electrical conductivity,which boosting the charge transfer kinetics.Therefore,the as-synthesized PPy exhibits a remarkable capacitance performance(7250 mF/cm^(2)@3 mA/cm^(2)),outstanding rate capability(3073 mF/cm^(2)@200 mA/cm^(2))and a long cycle life.The assembled symmetric and asymmetric supercapacitors(ASC)exhibit good energy densities(0.8 mWh/cm^(2) for ASC and 0.5 mWh/cm^(2) for symmetric supercapacitor),and excellent durability with zero capacitive loss after 35,000 cycles.In addition,we have fabricated small pouch devices,which can effectively operate a variety of electronic products(including the high-voltage 5 V smartphone,and tablet)and well withstand the external extreme tests during operation,demonstrating the quantitative investigation of the real-life application of aqueous supercapacitors.

关键词： dual-doping energy storage polypyrrole pouch-type device pseudocapacitive pulse-potential polymerization

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Facile synthesis of Co and Ce dual-doped Ni3S2 nanosheets on Ni foam for enhanced oxygen evolution reaction

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Nano Research 2020年第8期13卷 2130-2135页

作者： Xiaoxia Wu Tong Zhang Jiaxu Wei Pengfei Feng Xingbin Yan Yu Tang Laboratory of Clean Energy Chemistry and Materials State Key Laboratory of Solid LubricationLanzhou Institute of Chemical Physics Chinese Academy of SciencesLanzhou730000China State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

Nano Research volume 13,pages2130–2135(2020)Cite this article 376 Accesses 2 Citations Metrics details Abstract Developing efficient and stable oxygen evolution reaction(OER)electrocatalysts via doping strategy has well-documented for electrochemical water splitting.Herein,a homogeneous structure(denoted as Co/Ce-Ni3S2/NF)composed of Co and Ce dual doped Ni3S2 nanosheets on nickel foam was synthesized by a facile one-step hydrothermal method.Co and Ce dopants are distributed inside the host sulfide,thereby raising the active sites and the electrical conductivity.Besides,the CeOx nanoparticles generated by part of the Ce dopants as a cocatalyst further improve the catalytic activity by adding defective sites and enhancing the electron transfer.As a consequence,the obtained Co/Ce-Ni3S2/NF electrode exhibits better electrocatalytic activity than single Co or Ce doped Ni3S2 and pure Ni3S2,with low overpotential(286 mV)at 20 mA-cm^−2,a small Tafel slope and excellent long-term durability in strong alkaline solution.These results presented here not only offer a novel platform for designing transition metal and lanthanide dual-doped catalysts,but also supply some guidelines for constructing catalysts in other catalytic applications.

关键词： electrocatalyst oxygen evolution reaction dual-doping CeOx Ni3S2

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