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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Enhancement in the electrochemical stability at high voltage of high nickel cathode through constructing ultrathin LiCoPO4 coating

Jian Wei,Houfei Xiong,Hao Zhang,Xueting Li,Yanyi Liu,Zongmo Shi

The challenge of commercial layered-structure nickel-rich cathodes in lithium-ion batteries (LIBs) are the rapid capacity/voltage degradation at high rate capability and thermal runaway. The wide operational voltage range and excellent electrochemical stability of the coating material are key points to improve electrochemical performance and thermal stability at high voltage and high rate conditions. The uniformly olivine-type LiCoPO 4 (LCP) coatings were successfully prepared on the surface of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode combining sol–gel method and heat treatment. The capacity retention and operating voltage stability of the cathode at high cutoff voltage of 4.6 V were dramatically improved due to the ultrathin and stable interface is designed. The modified NCM811 exhibited a high cycling capacity of 157.7 mAh·g −1 at 5 C with a capacity loss of only 12.1 %. In high nickel cathode coating modification, LCP as the thinnest phosphate coating effectively improves the capacity decay of the cathode at high rate. The interface reconstruction provided a stable channel of Li + transport, which suppressed the cathode/electrolyte interface reaction to enhance the stability. The formation of strong covalent P O bonds at the interface significantly reduced the oxidizing activity on the NCM811 surface, further inhibiting the oxygen release and irreversible phase transition.

研究领域: 材料科学 · 能源存储与转换
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Journal of the American Chemical Society · 2025 · IF 15.6

In situ Detection of the Molecule-Crowded Aqueous Electrode–Electrolyte Interface

Shiqiang Wei,Hongwei Shou,Zheng-Hang Qi,Shuangming Chen,Yong Han,Shucheng Shi,Yixiu Wang,Pengjun Zhang,Jialin Shi,Zijun Zhang,Yuyang Cao,Changda Wang,Jiewu Cui,Xiaojun Wu,Zhi Liu,Li Song

Electrode–electrolyte interface plays a crucial role in determining the stability and behavior of electrochemical electrodes. Although X-ray photoelectron spectroscopy has been established as a powerful analytical technique for interface chemistry, the necessity for ultrahigh vacuum remains a significant obstacle to directly detecting dynamic interfacial evolution, particularly in aqueous environments. Here, we employ tender-energy ambient pressure X-ray photoelectron spectroscopy (AP-XPS) to bridge the gap between ultrahigh vacuum and near-atmospheric pressure, enabling an in-depth investigation of the molecule-crowded aqueous interface evolution in a Zn metal anode. The results demonstrate that the persistent presence of additive molecules effectively inhibits direct contact between reactive Zn and H2O, while also facilitating uniform Zn deposition. In situ optical microscopy observations and synchrotron radiation X-ray diffraction further verified the uniform and dense Zn deposition, attributed to lateral growth induced by the (002) crystal facet evolution. As proof of its effectiveness, batteries incorporating the Zn//Zn, Zn//Cu, and full cell with the additive demonstrate significantly improved stability and reversibility. This finding opens up new avenues for exploration of interfacial chemistry at the molecule level, offering insights into the design of highly stable metal anodes of aqueous ion batteries for practical applications.

CAS / MDL: 643-79-8
研究领域: 材料科学 · 电化学 · 表面科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

The spatiotemporal studies of the salt-hardening effect of the coacervates of nano-ions for aqueous super-ionic electrolytes with enhanced electrochemical stability

Binghui Xue,Yuan Liu,Weigang Sun,Yuling Liang,Panchao Yin

The application of aqueous electrolytes is generally limited by their narrow electrochemical window (ECW), which sets an intrinsic limit on the practical voltage and energy density of fabricated energy storage devices. Herein, the coacervates of nano-ions are proposed as aqueous lithium-ion electrolytes with both high ion conductivity and broadened ECW. The hybrid complex coacervates of 1 nm nano-anions, metatungstate ([W 12 O 40 ] 8− ), and polyethylene glycol (PEG) are studied for their unique salt-hardening effect. The framework of random percolated nano-ions interweaved by PEG chains is demonstrated from small angle X-ray/neutron scattering (SAXS/SANS) and micro-rheology measurements. The introduced extra Li + can complex with the PEG backbone for strengthened PEG/nano-ion interaction. The relaxation dynamics follows the model of sticky reptation by treating the binding of Li + as effective stickers and this leads to the observed salt hardening effect, e.g., enhanced viscosity with the increased LiCl concentrations. This hybrid coacervate exhibits excellent ionic conductivity (∼0.027 S/cm), and the super-ionic nature of ion conduction is demonstrated employing fractional Walden rule. Suggested from diffusion ordered spectroscopy studies, the water molecules confined in the framework of the coacervates show hindered diffusive dynamics and this contributes to the extended ECW (∼2 V), demonstrating its potential application as aqueous lithium electrolytes.

研究领域: 材料科学 · 电化学 · 纳米技术
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ADVANCED MATERIALS · 2025 · IF 26.8

Halogen Ion-Mediated Hydrothermal Synthesis of Diverse MXenes with Tailored Heterostructures

Hanchen Xu,Hongwei Shou,Ziwei Yan,Kefu Zhu,Chuanqiang Wu,Wei Jiang,Zhanfeng Liu,Shiqiang Wei,Jialin Shi,Hassan Akhtar,Changda Wang,Li Song

Two-dimensional transition metal carbides and nitrides (MXenes) have attracted significant attention due to their exceptional physicochemical properties. Despite extensive studies, efficient methods for the production of MXenes with precise structural control still remain a challenge, thus hindering their potential in many specific applications. Herein, a halogen ion-mediated hydrothermal approach is proposed for the controllable preparation of diverse MXenes and their heterostructures with well-defined interfacial architectures, demonstrating its potential as a high-throughput synthesis strategy. As proof of concept, Mo 2 C can be synthesized on a gram scale by employing NH₄F in the hydrothermal etching process of Mo 2 Ga 2 C. Subsequently, this approach is applied to various MXenes, including Ti 3 C 2 , V 2 C, and Nb 4 C 3 . Moreover, NH 4 X (X = Cl, Br, I) etchants combined with small-molecule intercalants enabled the targeted synthesis of MXene-based heterostructures, such as Mo 2 CT x @MoS 2 featuring ≈15 nm amorphous MoS 2 surface layers. Notable, the Mo 2 CT x (Br) heterostructure exhibited outstanding electrochemical stability, delivering a capacity of 465.5 mAh g⁻¹ after 300 cycles at 1 A g⁻¹, and achieving high coulombic efficiency of 99.8% during lithium-ion battery cycling. This work establishes a versatile and scalable platform for the synthesis of MXene-based materials, thus paving the way for accelerating their potential in various fields.

CAS / MDL: 7440-55-3
研究领域: 材料科学 · 纳米技术 · 电化学 · 无机化学
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 47 ·18524-18531 · IF 8.262

Core–shell rGO/SnO2@CF with wrinkled surface used as structural anode material: high tensile strength and electrochemical stability

Mengjie Feng,Shubin Wang,Jiping Yang,Boming Zhang

As one of the most promising structural anode materials, carbon fibers (CF) have gained much attention. One of the central problems in their application is retaining their tensile strength and simultaneously improving their electrochemical properties. Herein, we report reduced graphene oxide/SnO2@carbon fibers (rGO/SnO2@CF) with wrinkled surfaces, fabricated via a simple hydrothermal method followed by heat treatment. This material exhibits prominent tensile properties, improved reversible capacity, excellent cycling stability and significantly enhanced first cycle coulombic efficiency. Compared to the reversible capacity at the 20th cycle, the rGO/SnO2@CF retained 93.6% reversible capacity after 100 cycles at 50 mA g−1, corresponding to a capacity fading of only 0.08% per cycle. The Weibull scale parameter and shape parameter of rGO/SnO2@CF were up to 4.63 GPa and 7.87, respectively. Our measurements revealed that the positive influence of rGO effectively countervailed the negative influence of the hydrothermal process on the tensile strength; the interleaved structure of rGO/SnO2 prevented the dispersion degree of tensile strength from decreasing; the synergistic effect of rGO and SnO2 enhanced the properties of the carbon fibers, including the tensile strength and the electrochemical properties; the formed rGO network structure and bicontinuous electronic transport pathway are in favor of the cycling stability.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2012 · IF 3.832

Exploration on the possibility of Ni foam as current collector in rechargeable lithium-air batteries

Xianjun Liu,Deyu Wang,Siqi Shi

The electrochemically interfacial stability between Ni foam and organic electrolyte is studied under Ar and O 2 atmospheres, respectively. The potential of Ni foam cycled under Ar atmosphere does not reach 3.8   V vs. Li/Li + , and is finally stabilized at ∼3.4   V vs. Li/Li + . This phenomenon is the result of the electrolyte's continuous decomposition, which produces a thick layer of particles (0.8–1.2   μm) covered on Ni foam surface. Ni foam under O 2 atmosphere can be successfully cycled between 2.0 and 4.5   V vs. Li/Li + although there exist some precipitations on the surface, which originate from the electrolyte decomposition occurring at 4.2   V vs. Li/Li + in the initial charge. For the cycling between 2.0 and 4.0   V vs. Li/Li + , Ni foam surface almost keeps intact. Our results reveal that O 2 atmosphere significantly improves the electrochemical stability between Ni foam and electrolyte and thus enables Ni foam to work as current collector in rechargeable lithium-air battery .

CAS / MDL: 7440-02-0
研究领域: 材料科学 · 电化学
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ADVANCED MATERIALS · 2018 ·Vol. 31 ·期 6 ·1806272 · IF 21.95

A Universal Strategy for Constructing Seamless Graphdiyne on Metal Oxides to Stabilize the Electrochemical Structure and Interface

Fan Wang,Zicheng Zuo,Liang Li,Feng He,Fushen Lu,Yuliang Li

The structural and interfacial stabilities of metal oxides (MOs) are key issues while facing the volumetric variation and intensive interfacial polarization in electrochemical applications, including lithium-ion batteries (LIBs), supercapacitors, and catalysts. The growth of a seamless all-carbon interfacial layer on MOs with complex dimensions is not only a scientific problem, but also a practical challenge in these fields. Here, the growth of graphdiyne under ultramild condition is successfully implemented in situ for coating MOs of complex dimensions. The seamless all-carbon interface and conductive network are formed at the same time. This method cleverly avoids the structural degradation of MOs at a high temperature in the presence of traditional carbon materials. Under the protection of the high-quality graphdiyne layer, the samples as LIB anodes deliver high performances in terms of Coulomb efficiency, capacity, long-term retention, and structural and interfacial stabilities. Both experimental achievements and theoretical calculations demonstrate that the graphdiyne is a particular protection layer for MOs and plays a crucial role for preventing the structural and interfacial degradation of the electrode. Furthermore, the universality of this method will promote the potential applications of many promising MOs in other electrochemical fields.

研究领域: 材料科学 · 电化学 · 能源存储
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Energy Storage Materials · 2022 · IF 20.831

Covalent organic framework film protected zinc anode for highly stable rechargeable aqueous zinc-ion batteries

Jing Zhao,Yunpan Ying,Guiling Wang,Kedi Hu,Yi Di Yuan,Hualin Ye,Zhaolin Liu,Jim Yang Lee,Dan Zhao

Although aqueous zinc-ion batteries (ZIBs) have demonstrated great potential for large-scale energy storage, dendrite growth in the Zn metal anode leads to poor electrochemical stability and unsatisfactory cycling life, restricting widespread utilization of ZIBs. Herein, a zincophilic covalent organic framework (COF; TpPa-SO 3 H) film is fabricated via interfacial reaction to stabilize the Zn anode (TpPa-SO 3 H@Zn-foil). The sulfonic acid groups on the TpPa-SO 3 H film coordinate with Zn 2+ ions and regulate the uniform deposition of Zn 2+ ions to inhibit the dendrite formation. Additionally, the TpPa-SO 3 H can release abundant protons (H + ) and achieve a dynamic equilibrium with OH − , thereby adjusting the desolvation of [Zn(H 2 O) 6 ] 2+ to prevent secondary reactions. This work demonstrates that COF film-coated Zn anodes are a family of promising electrode candidates and provides inspiration to other fields of batteries, such as the material design for separator and electrolyte.

CAS / MDL: 1313-13-9
研究领域: 材料科学 · 能源存储技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Ultrafine Pt nanoparticles embedded in defective porous carbon for efficient hydrogen evolution reaction

Xianrong Liu,Kunjie Wang,Yongcheng Li,Yunsi Wang,Bingxin Liu,Peng Zhang,Benhua Xu

Platinum (Pt) is the state-of-the-art electrochemical catalyst for hydrogen evolution reaction (HER), but its commercial developments are restricted by scarcity and high cost. In this paper, defective porous carbon is obtained by removing the doped nitrogen atoms at high temperatures and ultrafine Pt nanoparticles were embedded in the defective porous carbon (Pt NPs/DPC) via a facile hydrothermal method . Benefiting from the synergistic effect of ultrafine Pt NPs and conductive substrate, Pt NPs/DPC catalyst exhibits high electrochemical activity with a low overpotential of 30 mV at 10 mA cm −2 and Tafel slope of 31 mV dec −1 and remarkable long-term electrochemical stability in acid solution, demonstrating HER performance superior to commercial 40 % Pt/C.

研究领域: 材料科学 · 电化学
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Surfaces and Interfaces · 2024 · IF 5.7

Construction of heterophase MoOx/Ru assisted by self-assembled carboxymethylcellulose-Ru3+ nanosheet for improved alkaline hydrogen evolution

Liming Zeng,Yongyang Zhu,Daifeng Wu,Dongxing Wang,Qing Zhou

The hydrogen evolution reaction (HER) in alkaline medium is much sluggish than that in acidic medium due to the limited water dissociation step, thus accelerating the water dissociation kinetics is critical. Herein, we designed a MoO x species-modified ruthenium nanoparticle catalyst (MoO x /Ru/C-3) based on the unique electrostatic interaction between carboxymethylcellulose sodium salt (CMC) and metal ions , where an heterophase structure is formed between MoO x and Ru. The obvious electronic interaction between them allows the formation of synergistic promotion relationship involving the water dissociation on MoO x and the adsorbed hydrogen recombination on Ru. At a metal loading of 6.98 μg Ru cm-2 geo, the overpotential of 82 mV is just required to reach a current density of 10 mA cm −2 , exhibiting a significantly better apparent electrochemical activity than Ru/C (98 mV) without introduction of MoO x , which demonstrates superior or comparable alkaline HER activity to the recently reported Ru-based electrocatalysts . Meanwhile, the overpotential for Ru/C increased by 113 mV after 24 h of chronopotentiometric test, whereas only 61 mV elevates for MoO x /Ru/C-3, and even just 98 mV generates after 120 h. Thereof, introduction of MoO x species into Ru matrix can also markedly improve the electrochemical stability. The proposed material construction strategy in this study provides a feasible idea for the rational design of highly cost-performance alkaline hydrogen evolution catalysts.

CAS / MDL: 12054-85-2 9004-32-4
研究领域: 材料科学 · 电化学
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DESALINATION · 2024 · IF 8.3

Enhancement of interfacial interaction between carbon and silver nanoparticles through co-doping with nitrogen and phosphorus

Yiyun Cao,Lvji Yan,Bichao Wu,Dun Wei,Baixue Ouyang,Peng Chen,Tingzheng Zhang,Justice Annor Asare,Yuxin Jiang,Yingjie He,Haiying Wang

The capacitive deionization technology has demonstrated its efficacy in removing chlorine-containing contaminants from water. However, the long-term and selective removal of Cl − remains a significant challenge. We present the synthesis of nitrogen‑phosphorus co-doped carbon composites embedded with silver-metal particles by incorporating N and P heteroatoms, which serve as effective anchoring sites for metallic Ag. The design of the electrode material ultimately enhances the electrochemical stability of silver by facilitating strong interactions between nitrogen and phosphorus with the silver and carbon substrates, respectively, forming stable chemical bonds. The electrode material exhibited excellent dechlorination performance, with a selectivity factor (Cl − versus SO 4 2− ) of up to 83.4 for Cl − in wastewater in a mixed solution and an adsorption capacity of 99.2 mg·g −1 for Cl − . Additionally, the silver-based selective dechlorination electrode achieved a desalination capacity of 77.7 mg·g −1 for Cl − in a single system and demonstrated remarkable stability over 100 cycles, retaining 93.99 % of its capacity. The present study demonstrates that introducing nitrogen and phosphorus can significantly enhance the cyclic stability of silver‑carbon electrodes, thereby facilitating the sustainable treatment of chlorinated wastewater.

研究领域: 环境科学 · 材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

NiFe2O4 @Co3O4 heterostructure with abundant oxygen vacancies as a bifunctional electrocatalyst for overall water splitting

Jie Zhu,Qian Zhang,Peng Zhao,Lin Chen,Sudong Yang,Qiang Yan,Hongmei Li

Exploring robust and high-performance bifunctional electrocatalysts for overall water splitting is crucial for converting electric power to hydrogen energy, especially for the flexible utilization of intermittent green energy resources. Herein, pine-needle-like NiFe 2 O 4 @Co 3 O 4 heterostructure nanoarrays with abundant oxygen vacancies were deposited onto nickel foam via hydrothermal reaction , cathodic electrodeposition , and CaH 2 reduction. The synergistic approach boosts the electrochemical activity of catalyst by improving conductivity, mass diffusion efficiency, and active site quantity. Accordingly, the optimal electrocatalyst exhibits outstanding catalytic activity with high electrochemical stability in an alkaline medium, providing low overpotentials of 251 mV and 77 mV respectively to achieve 10 mA·cm −2 for catalyzing OER and HER . Moreover, the as-fabricated bifunctional electrocatalyst only requires a cell voltage of 1.56 V to enable a current density of 10 mA·cm −2 for realizing water electrolysis, outperforming many other previously reported catalysts. This work provides an inspiration for developing open structure materials with synergistic effect, and demonstrates a feasible method to synthesis high-efficiency electrocatalysts for water splitting.

研究领域: 材料科学 · 能源科学
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