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ACS Applied Energy Materials · 2022 · IF 6.959

Co3O4 Quantum Dot-Catalyzed Lithium Oxalate as a Capacity and Cycle-Life Enhancer in Lithium-Ion Full Cells

Bolei Shen,Haojing Zhang,Yingjie Wu,Hao Jiang,Yanjie Hu,Chunzhong Li

The demand for lithium compensation materials is becoming urgent as energy density requirements increase. As next-generation anodes, mixed silicon and carbon (Si–C) materials are limited by low efficiency in the first cycle owing to the formation of a solid electrolyte interphase film. However, most compensation materials are water- and oxygen-sensitive and exhibit low electrochemical activity and decomposition efficiency. In this study, water- and oxygen-stable lithium oxalate (Li2C2O4) was developed to enhance the capacity and cycle-life of the lithium-ion battery. Various metal oxides were screened to improve the electrochemical activity of Li2C2O4. Co3O4 exhibited the strongest catalytic performance, and the catalytic mechanism of Co3O4 on Li2C2O4 was studied by density functional theory. Ultrasonic atomization drying was used to combine Co3O4 quantum dots (Co3O4-QDs) with Li2C2O4 for improved efficiency. The electrochemical activity of the modified Li2C2O4 improved, and the decomposition voltage decreased from 4.65 to 4.0 V. The modified Li2C2O4 exhibits catalytic activity, and it can be used in LiFePO4, which has weak catalytic activity; the decomposition efficiency in the LiFePO4 system increased from 34.16 to 99.10%. In the Si–C//LiFePO4 full battery system, the first cycle discharge capacity increased from 80 to 160 mA h g–1; the lost capacity of the first cycle was fully compensated for. Additionally, the CO2 produced by Li2C2O4 decomposition could inhibit the decomposition of the electrolyte, further improving the cycle performance of the battery.

研究领域: 材料科学 · 电化学 · 能源存储
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Carbon-negative valorization of biomass waste into affordable green hydrogen and battery anodes

Hanmin Yang,Anissa Nurdiawati,Ritambhara Gond,Shiwei Chen,Shule Wang,Bin Tang,Yanghao Jin,Ilman Nuran Zaini,Ziyi Shi,Wujun Wang,Andrew Martin,Reza Younesi,Linda Sandström,Pär G. Jönsson,Weihong Yang,Tong Han

The global Sustainable Development Goals highlight the necessity for affordable and clean energy, designated as SDG7. A sustainable and feasible biorefinery concept is proposed for the carbon-negative utilization of biomass waste for affordable H 2 and battery anode material production. Specifically, an innovative tandem biocarbon + NiAlO + biocarbon catalyst strategy is constructed to realize a complete reforming of biomass pyro-vapors into H 2 +CO (as a mixture). The solid residues from pyrolysis are upgraded into high-quality hard carbon (HCs), demonstrating potential as sodium ion battery (SIBs) anodes. The product, HC-1600-6h, exhibited great electrochemical performance when employed as (SIBs) anodes (full cell: 263 Wh/kg with ICE of 89%). Ultimately, a comprehensive process is designed, simulated, and evaluated. The process yields 75 kg H 2 , 169 kg HCs, and 891 kg captured CO 2 per ton of biomass achieving approx. 100% carbon and hydrogen utilization efficiencies. A life cycle assessment estimates a biomass valorization process with negative-emissions (−0.81 kg CO 2 /kg-biomass, reliant on Sweden wind electricity). A techno-economic assessment forecasts a notably profitable process capable of co-producing affordable H 2 and hard carbon battery anodes. The payback period of the process is projected to fall within two years, assuming reference prices of 13.7 €/kg for HCs and 5 €/kg for H 2 . The process contributes to a novel business paradigm for sustainable and commercially viable biorefinery process, achieving carbon-negative valorization of biomass waste into affordable energy and materials.

CAS / MDL: 9005-38-3
研究领域: 能源工程 · 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Mechanisms of microalgae-induced flocculation for urban water carbon-negative clarification

Jianing Xiu,Ziyong Ow,Yuning Zhao,Xiaohui Bai

Urban rivers or water bodies play an important role in improving the ecological environment. However, many of them are turbid and uncomfortable. In this study, five species of microalgae were isolated from different natural water and used to find their growth potential, flocculation ability, turbidity and nutrient removal ability and the flocculation mechanisms were investigated. The results showed that, three microalgae species, namely, Ankistrodesmus sp. WZ3A4, Coelastrella tenuitheca W6D5, Chlorella sorokiniana W6A3 can efficiently reduce the turbidity in natural water. Optical microscope and SEM observations revealed that they can attach the suspended particles to form flocs and display high turbidity-removal efficiencies (TRE) of 74.7 %, 82.6 %, 93.8 % respectively in natural turbid water. Chlorella sorokiniana W6A3 can even reduce the turbidity from 60.3 NTU to 3.73 NTU. Through EPS component analysis, TRE changes and surface characteristics before and after EPS extraction, Fourier transform infrared (FTIR) spectrum analysis, we found that the high turbidity-removal efficiency of these microalgae species was not closely related to charge neutralization, but greatly associated with the tightly bound EPS and the high relative hydrophobicity. Hydrophobic interaction and the adhesion of extracellular macromolecular polysaccharides have important effects on the flocculation of microalgae in natural turbid water. FTIR showed that microalgae with higher turbidity-removal efficiencies all had stronger stretching vibration near 1135 cm −1 . This study demonstrates that light-driven self-flocculating microalgae can clarify natural turbid water while converting atmospheric carbon dioxide into living biomass through light energy and proposes a novel and carbon-negative technology for restoring urban turbid water environments.

CAS / MDL: 108-95-2
研究领域: 环境科学 · 微生物学 · 水处理 · 生物技术
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AICHE JOURNAL · 2023 ·Vol. 70 ·期 4 ·e18319 · IF 3.7

Synergy of carbanion siting and hydrogen bonding in super-nucleophilic deep eutectic solvents for efficient CO2 capture

Meisi Chen,Wenjie Xiong,Weida Chen,Shangyu Li,Feng Zhang,Youting Wu

Carbanion-based ionic liquids are proposed and utilized as the key components for the construction of five super-nucleophilic deep eutectic solvents (SNDESs) in the paper. The super-nucleophilic nature of carbanion-based ionic liquids (ILs) is found to enable the capture of CO 2 with large absorption capacity. However, the absorption is very slow in the IL due to high viscosity. The synergy of carbanion siting and hydrogen bonding is found to enable high and fast absorption of CO 2 in [N 2222 ][CH(CN) 2 ]-ethylimidazole (Eim), and a synergistic absorption mechanism is proposed and validated from spectroscopic analyses and quantum calculations. The enthalpy change of CO 2 absorption in [N 2222 ][CH(CN) 2 ]-Eim is calculated to be −39.6 kJ mol −1 according to the thermodynamic model, and the moderate value implies that both absorption and desorption of CO 2 in the DES are favored and well balanced. The carbanion and hydrogen bond mediated by SNDESs provides a novel insight into the efficient CO 2 capture.

研究领域: 化学 · 环境科学
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CARBON · 2024 · IF 10.5

Confined graphitization induced pore generation for designing novel potassium-ion battery carbon anode with large capacity and ultra-long cycle life

Jieqi Chen,Haiyan Zhang,Bingbing Li,Xiaolin li,Jingxun Chen,Meng Ning,Zhenghui Li

Carbon is one of the most superior anode materials for K-ion batteries but faces the challenges of low capacity and poor cycle stability. In general, the K + storage capacity depends on the graphitized carbon layers and defective structure, while the cycle stability can be enhanced by constructing sufficient nanospace to alleviate the volume expansion during the potassiation/depotassiation process. However, the above structures are difficult to integrate into a single carbon material because graphitization often eliminates defects and pore structures. In this work, we find that ultrathin carbon sheets have a confined graphitization effect, which allows the carbon layer to orientationally arrange at a low heating-treatment temperature. More importantly, this orientational arrangement causes size shrinkage, inducing structural splitting on the faces of the carbon sheets and producing abundant defects and a large number of pores. Based on this, we obtain a novel carbon with highly graphitized, large-surface-area and defect-rich frameworks, which gives a K + storage capacity of 358 mAh g −1 , and after 4000 cycles, this carbon shows no obvious capacity degradation, with a capacity retention rate of nearly 100 %. Carbon anodes of K-ion batteries with such large capacity and long cycling life have rarely been achieved before.

CAS / MDL: 128-69-8 68-04-2
研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Novel strategies for constructing highly efficient silicon/carbon anodes: Chemical prelithiation and electrolyte post-treatment

Dan Hu,Caiyun Wu,Qiubo He,Shuju Zhang,Shiquan Wang,Rong Zeng,Yanqing Zhang,Jianwen Liu

Chemical prelithiation is an effective method to compensate for the loss of active lithium due to the formation of solid electrolyte interface, effectively addressing the issue of low initial coulombic efficiency (ICE) in silicon/carbon (Si/C) materials. Herein, the Si/C anode is prelithiated in a 1 M lithium-phenanthrene/2-methyltetrahydrofuran (Li-Phe/2-MTHF) solution in our work, and the prelithiated Si/C anode is followed by post-treatment with commercial electrolytes containing lithium difluorobis(oxalato)phosphate (LiDFBOP). The PSi/C-L 0.5 , originated from the reaction between residual Li-Phe/2-MTHF and the commercial electrolyte containing 0.5 wt% LiDFBOP, possesses the artificial SEI film, which not only contains a proper amount of LiF but also is rich in Li 2 C 2 O 4 and Li 3 P. Among them, LiF and Li 2 C 2 O 4 ensures the stability of the SEI film. Simultaneously, the synergistic effect of Li 3 P and LiF improves its Li + transport kinetics. Therefore, the ICE of PSi/C-L 0.5 reaches 92.50 %, and almost no drop in capacity occurs after 100 cycles at 0.5 A/g. Furthermore, the capacity stays steady at about 270 mAh/g through nearly 500 cycles at 1 A/g, achieving an impressive capacity retention rate of 97.8 %, significantly outperforming un-treated Si/C. This study offers new directions for constructing SEI films with stable structures and high Li + kinetics transport.

研究领域: 材料科学 · 电化学
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NANOTECHNOLOGY · 2020 ·Vol. 32 ·期 8 ·085403 · IF 3.551

Yolk-void-shell Si–C nano-particles with tunable void size for high-performance anode of lithium ion batteries

Chaoye Zhu,Yao Zhang,Zhihong Ma,Hui Wang,Gunnar L Sly

Silicon is a promising anode for new-generation lithium ion batteries due to high theoretical lithium storage capacity (4200 mAh g−1). However, the low conductivity and large volumetric expansion hamper the commercialization of the silicon anode. In this case, we present a yolk-void-shell Si–C anode (denoted as Si@Void@C), which is synthesized through nano-Si oxidation, surface carbonization and etching of SiOx. The void can be fabricated only by the self-generation and etching of SiOx layer on the Si surface, without the help of template materials. Moreover, the void size can be adjusted only by means of the annealing temperature, which can be easily and precisely operated. The Si@Void@C/rGO with void size of 5 nm offers a discharge capacity of 1294 mAh g−1 after 100 cycles at a current density of 500 mA g−1. These enhanced performances can be ascribed to an appropriate size (5 nm) of void space which sufficiently accommodates the silicon volume expansion and stabilizes the carbon shell. At the same time, the voids effectively inhibit the growth of the solid electrolyte interface layer by depressing the decomposition of the electrolyte on the surface of Si in Si@Void@C/rGO. Furthermore, interfaces between Si@Void@C particles and rGO sheets construct bridges for electrons' conduction. In general, the present work provides a viable strategy for synthesizing silicon–carbon anode materials with long life.

研究领域: 材料科学 · 能源存储技术
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Catalysts · 2023 ·Vol. 13 ·期 5 ·800 · IF 3.9

Influence of Cu/Al Ratio on the Performance of Carbon-Supported Cu/ZnO/Al2O3 Catalysts for CO2 Hydrogenation to Methanol

Zhong Xie,Jinpei Hei,Lei Cheng,Jing Li,Xiaojie Yin,Sugang Meng

CO2hydrogenation to methanol was conducted using a set of activated carbon-supported Cu/ZnO/Al2O3catalysts (CCZA) prepared by an incipient wetness impregnation approach. The effect of the Cu/Al ratio on the physicochemical properties of the catalysts, as well as their catalytic performance, were investigated. As Cu/Al ratio increased, the metallic Cu surface area displayed a reducing trend from 6.88 to 4.18 m2∙gcat−1, while the CO2adsorption capacity exhibited an increasing trend. Meanwhile, aluminum content will have an important effect on the catalysts’ reducibility and, thus, on their catalytic performance. The CCZA-2.7-de catalyst demonstrated the highest selectivity to methanol at 83.75% due to the excellent distribution and synergistic effect of copper and zinc. Although the CO2conversion of CCZA-2.2-de and CCZA-3.5-de exceeded 10%, the CH3OH selectivity was less than 60%, which may be attributed to the larger particle sizes of ZnO and poor interactions in Cu–Zn. The present study offers a novel approach to increase the number of active sites, optimize the activated carbon-aided Cu/ZnO/Al2O3catalyst’s composition, and finally elucidate the mechanism for CO2hydrogenation to methanol.Keywords:CO2hydrogenation;CuO/ZnO/Al2O3catalyst;methanol synthesis;carbon-supported catalyst;thermocatalysis

研究领域: 催化 · 化学工程 · 环境科学
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PHYSICS AND CHEMISTRY OF LIQUIDS · 2024 · IF 1.2

Volumetric properties of CO2-loaded and unloaded 3-amino-1- propanol/1-amino-2-propanol/3-dimethylamino-1-propanol + N, N-dimethylacetamide binary mixture at (288.15 to 323.15) K and 101 kPa

Shuting Wang,Xueli Zhou,Qingyuan Song,Yuhuan Chen,Fang Yang

In this work, the densities of CO2-loaded and unloaded alkanolamine (1) + N, N-dimethylacetamide (DMAC) (2) mixtures were determined at temperature of (288.15 to 323.15) K and 101 kPa. The alkanolamines were primary amines, 3-amino-1-propanol (3A1P) and 1-amino-2-propanol (1A2P), and tertiary amine, 3-dimethylamino-1-propanol (3DMA1P). There CO2-unloaded 3A1P/1A2P/3DMA1P + DMAC binary systems with the whole concentration and two CO2-loaded 3A1P/1A2P + DMAC systems with alkanolamine mass fraction of (0.2, 0.3 and 0.4) were investigated. Based on the density values of CO2-unloaded binary systems, the thermal expansion coefficient (αp), excess molar volume (VmE), and apparent molar volume (Vφ,i) were calculated and discussed in terms of intermolecular interactions and spatial structure. The VmE values were positive under the studied conditions and increased with the temperature, and the maximum followed the decreasing order of 1A2P + DMAC > 3DMA1P + DMAC > 3A1P + DMAC. Additionally, the VmE data were well fitted with the Redlich-Kister equation with a small standard deviation (σ ≤ 0.024). For the CO2-loaded systems, the density values were correlated with temperature and concentration using different empirical equations, and the average relative deviations (ARD%) were less than 0.299%.

CAS / MDL: 7223-38-3
研究领域: 化学热力学 · 物理化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2025 ·Vol. 172 ·期 3 ·030507 · IF 3.3

Three-Dimensional Cross-Linked Carboxymethyl Chitosan Binder for Si/C Anodes: Enhancing Cycling Stability and Performance in High-Energy Lithium-Ion Batteries

Junchao Sun,Jing Jiang,Jianjiang He,Lan Cao,Qingfu Wang

The silicon-carbon (Si/C) anode offers a significantly higher theoretical specific capacity compared to conventional graphite anodes, while also demonstrating reduced volume expansion and enhanced cycling stability compared to pure silicon anodes. Consequently, Si/C anodes have attracted considerable attention as promising candidates for next-generation high-energy lithium-ion battery anode materials. However, volume expansion remains a critical challenge, leading to the detachment of active materials from the current collector (copper foil) and adversely affecting cycling performance. In this study, we introduce diglycidyl ether (EG) as a cross-linking agent to synthesize a novel three-dimensional cross-linked carboxymethyl chitosan (CCS-EG) binder for Si/C600 anodes (theoretical specific capacity of 600 mAh g−1 at 0.1 C). Electrochemical testing reveals that the CCS-EG binder significantly improves the cycling stability of the Si/C anode, achieving a capacity retention rate of 88.68% after 400 cycles at a current density of 0.5 C, compared to only 67.71% for the anode using the linear carboxymethyl chitosan binder. Furthermore, CCS-EG offers advantages such as low cost, ease of preparation, and environmental sustainability, making it a promising candidate for commercialization as a binder in next-generation high-energy lithium-ion batteries.

CAS / MDL: 107-21-1
研究领域: 材料科学 · 能源科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Rapid synthesis and enhanced microwave absorption of carbon-supported high-entropy metal oxide

Bosen Lei,Ge Wang,Caiyong Li,Qikui Fan,Zhimao Yang,Yong Li,Cheng Zhou,Chuncai Kong

Complex preparation process and long annealing time of high-entropy metal oxide (HEO) limit its extensive application as microwave absorber at civil and military fields. Herein, a rapid synthesis method of mesocarbon microbeads (MCMB)-loaded spinel structure (FeCoCrNiMnCu)O is studied via plasma flow. In the presence of extreme plasma heating rate, a nanoscale high-entropy phase can be formed while modifying the surface activity of carbon. Simultaneously, due to the short synthesis time, gaseous conversion of carbon under high temperature aerobic conditions is avoided. By appending of carbon, the dual-media absorber exhibits better absorption performance with a maximum peak (-44.7 dB), which achieves over 90 % absorption in 11.2–15.5 GHz with a thickness of only 1.9 mm. Interestingly, the real and imaginary parts of complex permittivity increase remarkably. The former change is attributed to the expansion of heterogeneous hole carrier region and the latter dues to the interfacial polarization of the strongly coupled interface. The increase of dielectric loss and conductance loss leads to great improvement of microwave absorption. Our study injects new vitality into the preparation of HEO for advanced applications and the as-prepared HEOM is promised to be high-efficient microwave absorber based on robust stability and excellent absorbing performance.

研究领域: 材料科学 · 电磁学
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 32 ·期 33 ·2203279 · IF 19.924

Boosting Surface-Dominated Sodium Storage of Carbon Anode Enabled by Coupling Graphene Nanodomains, Nitrogen-Doping, and Nanoarchitecture Engineering

Si Huang,Dongjie Yang,Xueqing Qiu,Wenli Zhang,Yanlin Qin,Caiwei Wang,Conghua Yi

The development of high-performance carbon anode for sodium-ion batteries is limited by the sluggish kinetics and structural instability. Expanded interlayer spacing, nitrogen doping, and mesoporous structure engineering have emerged as promising strategies to overcome these challenges. Simultaneously achieving graphene nanodomains construction, high-efficient nitrogen doping, and rational mesoporous structure engineering is challenging. Herein, a strategy of pyrolyzing SiO 2 @ lignin amine urea-formaldehyde resin is proposed for deliberate manipulation of graphene nanodomains, edge-nitrogen doping, and specific mesoporous distribution in amorphous lignin-derived carbon based on polycondensation-template. The obtained carbon material exhibits a nitrogen-doping level of 6.03 at% with a high edge-nitrogen ratio of up to 84.4%, high- connectivity mesoporous structure, and graphene nanodomains with expanded interlayer spacing. The optimized carbon material delivers a reversible capacity of 234 mAh g −1 at 100 mA g −1 , superior rate capability of 129 mAh g −1 at 2 A g −1 , and excellent cycling stability. In addition, the surface-dominated sodium-ion storage mechanism is identified by in situ electrochemical impedance spectroscopy. Furthermore, the optimized carbon can function as an outstanding anode for full cells. This work proposes a new avenue for designing high-performance carbon for low-cost and high-rate sodium-ion batteries.

研究领域: 材料科学 · 电化学
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