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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 38 ·26076-26082 · IF 10.7

Relaxing the Jahn–Teller distortion of LiMn0.6Fe0.4PO4 cathodes via Mg/Ni dual-doping for high-rate and long-life Li-ion batteries

Haifeng Yu,Erdong Zhang,Jinxun Yu,Songmin Yu,Yaoguo Fang,Ling Chen,Hao Jiang,Chunzhong Li

Olivine-type LiMnxFe1−xPO4 (LMFP, 0 < x < 1) is poised to supplant LiFePO4 cathode materials with a ∼20% energy-density increase for Li-ion batteries (LIBs). However, its intrinsic low conductivities and MnO6 octahedral unit-cell Jahn–Teller distortion limit its power capability and cycling life. Herein, we report a Mg/Ni dual-doped and carbon-coated LMFP micro-sized secondary sphere with greatly enhanced reaction kinetics and superior structure stability. Ni2+ reduces the average valence state of Mn ions to alleviate Jahn–Teller distortion by participating in charge compensation during charging while improving electronic conductivity together with carbon coating. Mg2+ with a smaller ion radius (65 pm) significantly widens the Li-ion transfer channel by extending Li–O bonds. The as-obtained LMFP cathodes increase reversible specific capacity by about 2.4 times at 5C compared with a pristine sample, reaching 115 mA h g−1. In a pouch-type full cell, 92% of its initial capacity is still maintained after 2000 cycles at 1C, demonstrating its attractive potential for practical application in high-power and long-life LIBs.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Enhancement of La–Ti modification on the conductivity and stability of Co-free Li- and Mn-rich layered cathode

Wei Liu,Xin Geng,Hailong Wang,Jing Chen,Chenyang Wang,Nian Zhang,Ahmed M. Hashem,Wei Chu,Xin He

Lithium (Li) - and manganese (Mn)-rich oxides ( x Li 2 MnO 3 ·(1− x ) Li TM O 2 , TM  = Ni, Co, Mn, etc.) are one of the most promising cathode materials because of their high theorical capacity, which is contributed by the redox of both transition metal cations and oxygen anion. However, anionic redox leads to transition-metal migration and release of lattice oxygen, which further triggers voltage decay and capacity fade. Here, we report a dual-doping and multiphase co-existence strategy to tackle the structure degradation of Li- and Mn-rich materials and enhance electrochemical kinetics. La–Ti dual cations doping strength the TM -O bonds and improve cycling stability, and the inducement of LaMnO 3+ δ (LaMO) phase provides higher conductivity. As a result, the unique architecture presents a favourable rate performance, improved capacity retention, and suppressed voltage decay. After 200 cycles at 1C (250 mA g −1 ), the La–Ti dual cations doped Li-and Mn-rich material shows 24 % higher capacity retention and 52 % lower voltage decay compared to the non-doped material. This study demonstrates the potential of dual transition-metal ion doping combined with doping-induced perovskite phase to enhance the performance of Li- and Mn-rich materials.

CAS / MDL: 554-13-2 10277-43-7
研究领域: 材料科学 · 能源存储技术
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Texturing In-Situ: N/F Dual-Doped hollow porous carbon nanospheres for advanced Li-S batteries

Jinlong Hu,Qingqing Chen,Qi Xia,Lingzhi Zhang

Heteroatom-doped hollow carbon nanostructures are one of the most promising sulfur hosts for high-performance lithium-sulfur (Li-S) batteries. However, finding a facile and controllable synthesis and enhancing their immobilization effect on polysulfides have been challenging. Herein, we propose a one-step in-situ reaction approach to synthesize N/F dual-doped hollow micro/mesoporous carbon nanospheres (NFHCs) as multifunctional sulfur host, which integrates the physical confinement of hollow porous structure and chemical adsorption/catalytic ability of N/F active sites to realize strong anchoring and accelerated conversion of polysulfides. This sulfur cathode based on NFHCs host with a high sulfur content of 80 wt% enables a superior high-rate capacity of 689 mAh g −1 at 3C, accompanied by outstanding cycle life over 500 cycles at 2C with a capacity decay of only 0.05% per cycle and nearly 100% Coulombic efficiency. This work opens up new horizons to design nanostructured functional hollow carbons for advanced Li-S batteries.

研究领域: 材料科学 · 能源存储
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Sulfur/nitrogen dual-doped three-dimensional reduced graphene oxide modified with mesoporous TiO2 nanoparticles for promising lithium-ion battery anodes

Jinghao Huo,Yijie Ren,Yujia Xue,Yi Liu,Shouwu Guo

Three-dimensional graphene is often used as electrode materials due to its excellent electrochemical properties . In this work, sulfur/nitrogen dual-doped reduced graphene oxide (SNG) foam is prepared by a simple sol-gel method with l -cysteine. Furthermore, mesoporous dioxide-titanium (TiO 2 ) nanoparticles are deposited on the surface of SNG at 60 °C to improve the Li + ions diffusion kinetics. As an anode material for lithium ion batteries , the SNG/TiO 2 has an excellent reversible discharging capacity (444 mAh g −1 , 0.1 A g −1 ) and good rate capability (217 mAh g −1 , 2.0 A g −1 ). In addition, the SNG/TiO 2 electrode delivers a specific capacity as high as 148.8 mAh g −1 at a current density of 1.0 A g −1 after 1000 cycles, and even at a high current density of 5.0 A g −1 , a reversible capacity of 99 mAh g −1 can also be achieved. Hence, the SNG/TiO 2 composite synthesized by a simple template-free method at a low-temperature is a promising anode material for lithium ion batteries.

CAS / MDL: 52-90-4
研究领域: 材料科学 · 能源科学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2020 · IF 3.807

Fe, N dual doped graphitic carbon derived from straw as efficient electrochemical catalysts for oxygen reduction reaction and Zn-air batteries

Jianpeng Li,Xianfeng Li,Hongyan Chen,Dingshu Xiao,Jiajia Li,Dekang Xu

In this paper, we present a facile and one-step way for synthesizing Fe, N dual doped highly porous graphitic biomass carbon (FeNC) by using K 2 FeO 4 to fulfill the activated process and catalytic graphitization of straws. The FeNC demonstrates hierarchically porous structure with large surface area of 1034 m 2 g −1 , Fe, N dual doping with certain amount of Fe-N x , and graphitic structure. With these favorable features, the electrocatalytic activity for oxygen reduction reaction (ORR) reveals that the FeNC exhibits positively onset potential with highly comparable limiting current density when comparing with the sample using conventional KOH activated agent. In additional, the assembled Zn-air battery using FeNC as air-cathode catalyst delivers a maximal power density of 128.4 mW cm −2 . Considering the abundance of straws on the earth and the low-cost and green prepared process, the present FeNC materials are highly promising in application in ORR catalysts for Zn-air battery and other energy-related fields.

CAS / MDL: 7440-06-4
研究领域: 材料科学 · 能源化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Hierarchical self-assembled SnS@N-S dual-doped carbon microflower spheres as anode for high performance lithium-ion batteries

Shuyun Wan,Xi Liu,Likang Fu,Chengbao Zhou,Hongyi Chen,Guanghui Li,Shiyue Cao,Qiming Liu

Stannous sulfide (SnS) with low-cost and high theoretical specific capacity possesses enormous potential in the application of lithium-ion batteries (LIBs). However, the sluggish Li ion diffusion kinetics and severe volume variation of SnS, result in inferior rate capability and poor cycling stability. Hollow SnS microflower spheres coated with N, S dual-doped carbon (H-SnS@NSC) are constructed through a facile hydrothermal reaction , polydopamine encapsulation and subsequent carbonization process. Such rational hollow structure is conducive to enhance the structural stability of the material. More importantly, N, S dual-doped carbon is synergistically coupled with SnS, which can greatly improve the electrons/ions kinetics and mitigate the volume expansion. As consequence, the H-SnS@NSC composite electrode exhibits an admirable specific capacity of 778.5   mAh   g −1 at 0.5 A g −1 after 400 cycles. It still remains a specific capacity of 633.8   mAh   g −1 after 800 cycles even at 1.0 A g −1 , corresponding to 81.7% of initial capacity. After being assembled into a full cell, the device delivers a stable capacity of 317   mAh   g −1 at 0.1 A g −1 . This work manifests that morphology and structure engineering have bright prospects in promoting the practical applications for metal sulfides.

CAS / MDL: 7439-93-2
研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Template-free construction of hollow mesoporous carbon spheres from a covalent triazine framework for enhanced oxygen electroreduction

Yong Zheng,Shan Chen,Kai A.I. Zhang,Jingyu Guan,Xiaohui Yu,Wei Peng,Hui Song,Jixin Zhu,Jingsan Xu,Xiaoshan Fan,Chao Zhang,Tianxi Liu

The construction of hollow mesoporous carbon nanospheres (HMCS) avoiding the use of traditional soft/hard templates is highly desired for nanoscience yet challenging. Herein, we report a simple and straightforward template-free strategy for preparing nitrogen, sulfur dual-doped HMCSs (N/S-HMCSs) as oxygen reduction reaction (ORR) electrocatalysts. The unique hollow spherical and mesoporous structure was in-situ formed via a thermally initiated hollowing pathway from an elaborately engineered covalent triazine framework. Regulation of pyrolysis temperatures contributed to precisely tailoring of the shell thickness of HMCSs. The resulting N/S-HMCS 900 (pyrolyzed at 900 °C) possessed high N and S contents, large specific surface areas, rich and uniform mesopores distribution. Consequently, as a metal-free ORR electrocatalyst, N/S-HMCS 900 exhibits a high half-wave potential, excellent methanol tolerance and great long-term durability. Additionally, density functional theory calculations demonstrate that N, S-dual dopant can create extra active sites with higher catalytic activity than the isolated N -dopant. This strategy provides new insights into the construction of hollow and mesoporous multi-heteroatom-doped carbon materials with tunable nanoarchitecture for various electrochemical applications.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Novel Research Approach Combined with Dielectric Spectrum Testing for Dual-Doped Li7P3S11 Glass-Ceramic Electrolytes

Nan Zhang,Fei Ding,Shihui Yu,Kongying Zhu,Huan Li,Weiguo Zhang,Xingjiang Liu,Qiang Xu

Owing to the expanding function of Li-ion transmission channels, it is important to explore the doping effects of different compounds into sulfide solid electrolytes to improve their electrochemical performances. However, it is hard to characterize the doping behaviors within sulfide solid electrolytes with low crystallinity and poor stability just by conventional crystallography analytical methods. In this work, the dielectric spectrum testing combined with other analytical methods, such as 7Li solid-state nuclear magnetic resonance, X-ray photoelectron spectroscopy, and the electrochemical method, have been applied to investigate the dual-doping behaviors of WS2 and LiBr within Li7P3S11 glass-ceramic electrolytes. This research method can not only evaluate the internal acting effect between the skeleton of sulfide solid electrolytes and the migrating kinetics of Li ions but also explore the capacitance at the interfaces of LiCoO2/sulfide solid electrolytes. The experimental results show that the number of Li ions with fast transport velocity within Li2S-P2S5-based solid electrolytes has been increased. Meanwhile, the interfacial capacitances between Li2S-P2S5-based solid electrolytes and the LiCoO2 cathode have decreased after dual-doping of WS2 and LiBr, indicating a synergetic effect for the doped Li7P3S11 glass-ceramic electrolytes in terms of the ionic conductivities and interfacial compatibilities. This work may provide a novel analytical approach to explore both the diffusion kinetics and interfacial behaviors for the solid electrolytes of lithium batteries.

研究领域: 材料科学 · 电化学
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Small · 2024 · IF 13

Dual-Doping Strategy for Lowering the Thermal Expansion Coefficient and Promoting the Catalytic Activity in Perovskite Cobaltate Air Electrodes for Solid Oxide Cells

Shuxiong Wang,Xiaoxin Zhang,Yu Chen,Fan Fan,Chang Jiang,Yongkang Xiang,Xiao Xiao,Yuan Fang,Abdullah N. Alodhayb,Jianhui Li,Jijie Huang,Yifei Sun,Zhou Chen

Lowering the thermal expansion coefficient (TEC) and promoting the catalytic activity of cobalt-based perovskite air electrodes is crucial for efficient solid oxide cells (SOCs) devices. However, the co-achievement of both merits has usually been largely compromised in most scenarios. Herein, a dual-doping strategy to manipulate the properties of perovskite cobaltate electrocatalyst is reported in which a high valence element of Ta 5+ is incorporated into B-site to significantly suppress the dynamic reduction of Co 4+ species and reduces the TEC value from PrBaCo 2 O 5+δ (PBC, 17.8 × 10 ⁻6 K −1 ) to PrBaCo 1.96 Ta 0.04 O 5+δ (PBCT, 12.5 × 10⁻ 6 K −1 ) and suppresses the oxygen loss in SOCs operation condition, revealing the improved structural stability. Meanwhile, the Ca 2+ is doped into A-site of Ta-incorporated candidate, further decreasing the covalency of Co─O bonds and facilitating the formation of oxygen vacancies, benefiting the oxygen exchange kinetics and leading to a low polarization resistance of 0.026 Ω cm 2 (800 °C) in as-prepared PrBa 0.8 Ca 0.2 Co 1.96 Ta 0.04 O 5+δ (PBCCT) electrode. The cell with PBCTT demonstrates remarkable robustness during a 50 h thermal cycling test (25 cycles). Moreover, it delivers a high current density of 1.44 A cm⁻ 2 (1.6 V, 800 °C), as well as attractive durability over 100 h for pure CO 2 electrolysis.

研究领域: 材料科学 · 电化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2018 · IF 5.667

Low-temperature rapid synthesis of nitrogen and phosphorus dual-doped carbon dots for multicolor cellular imaging and hemoglobin probing in human blood

Shan Huang,Erli Yang,Yi Liu,Jiandong Yao,Wei Su,Qi Xiao

Heteroatom doping of carbon dots (CDs) can efficiently tune the structure of electronic energy levels and modulate the photochemical properties of CDs. However, the reported synthesis routes of heteroatom-doped CDs are complicated and rigorous. Herein, a simple and rapid low-temperature heating strategy was applied to synthesize fluorescent nitrogen and phosphorus dual-doped CDs (N,P-CDs) using sucrose as carbon source, and 1,2-ethylenediamine (EDA) and phosphoric acid as dopants, respectively. These N,P-CDs exhibit excellent fluorescent stability over wide pH range solutions (4–11), ultrahigh ion strength (3 M KCl), and longtime UV light irradiation (3 h continuously), which makes these N,P-QDs promising good candidates for fluorescent probes. These N,P-CDs showed excellent biocompatibility, multicolor cellular imaging, and non-cytotoxicity to human hepatocellular carcinoma HepG2 cells even at 500 μg/mL levels for 48 h incubation. These N,P-CDs exhibited a strong blue emission and a sensitive response to hemoglobin. The N,P-CDs based fluorescent probe was then applied to sensitively determine hemoglobin with a detection limit of 0.29 nM. Notably, it was also applied for label-free detection of hemoglobin in human urine samples and human blood samples, which indicated its potential applications in clinical diagnosis and other biologically related study.

研究领域: 生物医学工程 · 分析化学 · 纳米材料科学
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ENERGY · 2023 · IF 9

High nitrogen-oxygen dual-doped three-dimensional hierarchical porous carbon network derived from Eriocheir sinensis for advanced supercapacitors

Yunchao Li,Yangkai Sun,Hanming Li,Mengwei Sun,Jie Shen,Shurong Wang

In this study, we report a unique, facile process for the preparation of a high-nitrogen-oxygen dual-doped three-dimensional (3D) hierarchical porous carbon network by one-step pyrolysis and in situ activation under a CO 2 atmosphere combined with acid treatment using Eriocheir sinensis as the precursor. The evolution of the physicochemical structure of carbon at different pyrolysis temperatures was investigated. Removing inorganics from the shell carbon of Eriocheir sinensis enabled the formation of a unique 3D network structure. In addition, a high doping concentration of nitrogen and oxygen can be formed in the porous carbon skeleton. The increase in the pyrolysis temperature was beneficial to the pore development and graphitisation of carbon. Because of the interconnected 3D hierarchical porous structure and high heteroatom doping content, which provides fast channels for electron and ion transport, the obtained carbon materials exhibit excellent capacitive performance as supercapacitor electrodes. Quantum chemical calculations further confirmed that the heteroatom-doped carbon plane has a larger negative charge and stronger interaction with K + than that of the pure carbon surface. This inexpensive green carbon material based on food waste is expected to be a candidate material for high-performance electrode precursors.

CAS / MDL: 9002-84-0
研究领域: 材料科学 · 能源存储
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Densified graphene-like carbon nanosheets with enriched heteroatoms enabling superior gravimetric and volumetric potassium storage capacities

Chunliu Zhu,Xuehui Wang,Lei Yang,Zongying Gao,Weiqian Tian,Jingwei Chen,Jing Shi,Shuai Liu,Minghua Huang,Jingyi Wu,Huanlei Wang

Constructing carbon electrodes with abundant heteroatoms and appropriate graphitic interlayer spacing remains a major challenge for achieving high gravimetric and volumetric potassium storage capacities with fast kinetics. Herein, we constructed 3D graphene-like N, F dual-doped carbon sheets induced by Ni template (N, F-CNS-Ni) with dense structure and rich active sites, providing a promising approach to address the facing obstacles. Highly reversible K-ion insertion/extraction is realized in the graphitic carbon structure, and K-adsorption capability is enhanced by introducing N/F heteroatoms. As a result, the N, F-CNS-Ni electrode exhibits ultrahigh gravimetric and volumetric capacities of 404.5 mA h g −1 and 281.3 mA h cm −3 at 0.05 A/g, respectively, and a superb capacity of 259.3 mA h g −1 with a capacity retention ratio of 90 % even after 600 cycles at 5 A/g. This work presents a simple Ni-based template method to prepare graphene-like carbon nanosheets with high packing density and rich heteroatoms, and offers mechanism insight for achieving superior K-ion storage.

CAS / MDL: 75-05-8
研究领域: 材料科学 · 能源存储
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