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Journal of Energy Chemistry · 2025 · IF 14.9

Alloy-type Mo single-atom catalyst enhancing hydrogen storage performance of MgH2

Cenyu Yang,Chen Hu,Xiaoyu Wu,Yao Pang,Xiaofang Liu,Jianglan Shui

Metallic single-atom catalysts (SACs) have demonstrated high activity and potential in enhancing the hydrogen storage properties of MgH 2 . However, previous reports primarily focus on supported SACs, which often suffer from insufficient contact between single-atom active sites and hydrogen storage materials. In this study, the precursor Mo(CO) 6 is uniformly dispersed on the surface of MgH 2 via impregnation adsorption, leading to the formation of alloy-type Mo single atoms after hydrogenation/dehydrogenation activation. This alloy structure enables zero-distance contact between catalytic sites and the hydrogen storage material, facilitating electron exchange and hydrogen transfer between the Mo sites and MgH 2 . The MgH 2 loaded with Mo single atoms (Mo 1 -MgH 2 ) exhibits excellent hydrogen absorption and desorption properties, with the initial hydrogen release temperature lowered from 323 to 218 °C. At 250 °C, Mo 1 -MgH 2 absorbs over 6.77 wt% of hydrogen within 1 min and releases over 5.85 wt% within 4 h. During 10 cycles of hydrogenation and dehydrogenation reactions, Mo 1 -MgH 2 maintains nearly 100% capacity and shows stable kinetics. This work provides new insights into the design and fabrication of catalysts for hydrogen storage materials.

CAS / MDL: 13939-06-5
研究领域: 材料科学 · 催化化学
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ACS Nano · 2022 · IF 18.027

Alloy-Type Lithium Anode Prepared by Laser Microcladding and Dealloying for Improved Cycling/Rate Performance

Li Cao,Min Zheng,Jingbo Wang,Songyuan Li,Jiejie Xu,Rongshi Xiao,Ting Huang

Nanosized alloy-type materials (Si, Ge, Sn, etc.) present superior electrochemical performance in rechargeable batteries. However, they fail to guarantee cycling capacity and stability under high mass loading required by industrial applications due to low electric contact and adhesive strength, which has long been a challenge. This work proposes a rational design for an alloy-type anode via facile and versatile laser microcladding and dealloying. The proposed anode features a large-area porous network composed of continuous nano-ligaments, which consist of evenly distributed nanosized alloy-type material metallurgically bonded with conductive material. The fabrication of the structure is validated using Ge–Cu and Sn–Cu anodes, both exhibiting enhanced cycling stability at high areal capacity and rate performance in lithium-ion batteries. The enhancement is attributed to the structural features, which contribute to lithiation–delithiation stability and intact electron/Li ion transference path, as verified by in situ and ex situ transmission electron microscopy observations. More importantly, the critical solidification conditions of laser microcladding are provided by a multiphysics simulation, allowing for a thorough understanding of the structural formation mechanism. The study provides a possible approach to improve mass loading and performance of an alloy-type anode for practical application.

研究领域: 材料科学 · 能源存储
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Pb nanospheres encapsulated in metal–organic frameworks-derived porous carbon as anode for high-performance sodium-ion batteries

Xiaoying Zhao,Ningbo Liu,Chaonan Mu,Bin Qin,Liubin Wang

Alloying-type anode materials are considered promising candidates for sodium-ion batteries (SIBs) due to their high theoretical capacities. However, their application is limited by the severe capacity decay stemming from dramatic volume changes during Na + insertion/extraction processes. Here, Pb nanospheres encapsulated in a carbon skeleton (Pb@C) were successfully synthesized via a facile metal–organic frameworks (MOFs)-derived method and used as anodes for SIBs. The nanosized Pb particles are uniformly incorporated into the porous carbon framework, effectively mitigating volume changes and enhancing Na + ion transport during discharging/charging. Benefiting from this unique architecture, a reversible capacity of 334.2 mAh g −1 at 2 A g −1 is achieved after 6000 cycles corresponding to an impressive 88.2 % capacity retention and a minimal capacity loss of 0.00748 % per cycle. Furthermore, a high-performance full sodium-ion battery of Pb@C//NVPF was constructed, demonstrating a high energy density of 291 Wh kg −1 and power density of 175 W kg −1 . This facile MOFs-derived method offers insights into the design of high-capacity alloy-type anode materials using Pb sources, opening up new possibilities for innovative approaches to Pb recycling and pollution prevention.

研究领域: 材料科学 · 能源存储与转换
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Journal of Energy Chemistry · 2022 · IF 13.599

Bi nanoparticles in situ encapsulated by carbon film as high-performance anode materials for Li-ion batteries

Jun Yang,Jiahui Xian,Qinglin Liu,Yamei Sun,Guangqin Li

Bismuth (Bi) has indeed inspired great interests in lithium-ion batteries (LIBs) due to the high capacity, but was still limited by the low electrical conductivity and large volume variation. Herein, a composite material based on Bi nanoparticles in situ encapsulated by carbon film (Bi@CF) is prepared successfully through a facile metal–organic framework (MOF)-engaged approach. As anode materials for LIBs, the Bi@CF composites achieved high reversible capacities of 705 and 538 mAh g −1 at 0.2 and 0.5 A g −1 after 200 cycles, and long cycling performance with a stable capacity of 306 mAh g −1 at 1.0 A g −1 even after 900 cycles. In situ X-ray diffraction (XRD) measurements clearly revealed the conversion between Bi and Li 3 Bi during the alloying/dealloying process, confirming the good electrochemical reversibility of Bi@CF for Li-storage. The reaction kinetics of this Bi@CF composite was further studied by galvanostatic intermittent titration technique (GITT). This work may provide an inspiration for the elaborate design and facile preparation of alloy-type anode materials for high-performance rechargeable batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Sb nanocrystallites derived from industrial antimony white as promising alloying-type anodes for Na-ion batteries

Yunhao Zhu,Jie Shao,Yu Jiang,Kejia Zhang,Qiang Shi,Qunting Qu,Honghe Zheng

Alloying-type anodes exhibit unique advantages in terms of capacity and working potentials for practical application in sodium-ion batteries (SIBs). Sb-based nanocrystallites are prepared through a low-cost and large-scalable route by reducing the industrial antimony white (Sb 2 O 3 ) in aqueous solutions under mild conditions and studied as the anode materials of SIBs. Compared with the pristine Sb 2 O 3 and partially reduced Sb/Sb 2 O 3 hybrid, the totally reduced product (pure Sb nanocrystallite) manifests the most steady desodiation potential, highest capacity at around 0.75 V vs. Na + /Na, highest initial Coulombic efficiency, longest cycling life, and fastest charge/discharge rate. The different electrochemical performance of as-prepared materials is discussed from the perspective of Na-storage mechanisms. The results demonstrate that the as-prepared pure Sb nanocrystallite is more promising than its oxides for practical application in SIBs.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

NiM (Sb, Sn)/N-doped hollow carbon tube as high-rate and high-capacity anode for lithium-ion batteries

Chaocang Weng,Sumei Huang,Ting Lu,Junfeng Li,Jinliang Li,Jiabao Li,Likun Pan

Alloy-type materials are regarded as prospective anode replacements for lithium-ion batteries (LIBs) owing to their attractive theoretical capacity. However, the drastic volume expansion leads to structural collapse and pulverization, resulting in rapid capacity decay during cycling. Here, a simple and scalable approach to prepare NiM (M: Sb, Sn)/nitrogen-doped hollow carbon tubes (NiM C) via template and substitution reactions is proposed. The nanosized NiM particles are uniformly anchored in the robust hollow N -doped carbon tubes via Ni N C coordination bonds, which not only provides a buffer for volume expansion but also avoids agglomerating of the reactive material and ensures the integrity of the conductive network and structural framework during lithiation/delithiation. As a result, NiSb C and NiSn C exhibit high reversible capacities (1259 and 1342 mAh/g after 100 cycles at 0.1 A/g) and fascinating rate performance (627 and 721 mAh/g at 2 A/g), respectively, when employed as anodes of LIBs. The electrochemical kinetic analysis reveals that the dominant lithium storage behavior of NiM C electrodes varies from capacitive contribution to diffusion contribution during the cycling corresponding to the activation of the electrode exposing more NiM sites. Meanwhile, M (Sb, Sn) is gradually transformed into stable NiM during the de-lithium process, making the NiM C structure more stable and reversible in the electrochemical reaction. This work brings a novel thought to construct high-performance alloy-based anode materials.

研究领域: 材料科学 · 电化学
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Advanced Energy Materials · 2022 ·Vol. 13 ·期 9 ·2202939 · IF 29.698

Intermolecular Cross-Linking Reinforces Polymer Binders for Durable Alloy-Type Anode Materials of Sodium-Ion Batteries

Qian Yao,Yansong Zhu,Cheng Zheng,Nana Wang,Dongdong Wang,Fang Tian,Zhongchao Bai,Jian Yang,Yitai Qian,Shixue Dou

Sodium-ion batteries show promising potential for large-scale energy storage. However, the large size and heavy mass of Na + always results in huge volume change and inferior electrochemical stability, especially in alloy-type anode materials. Here, molecular engineering of the polymer binders, i.e., cross-linking of poly(acrylic acid) with glycerin (PAA-GLY), reinforces the mechanical properties, eliminates the active protons of PAA, and benefits electrolyte diffusion, thereby remarkably improving electrochemical performance. Using µ-Sn as an example, the cycle life at 2 A g −1 is extended from ≈26 cycles of PAA to ≈2000 cycles of PAA-GLY. Meanwhile, the initial Coulombic efficiency is promoted to 90.3%, allowing the fabrication step of electrode presodiation for full cells to be eliminated. Thus, the full cells run 300 cycles at 2 A g −1 . In addition, the binder allows the thick electrode to exhibit an areal capacity of 6.8 mAh cm −2 . This binder is also applied for µ-Bi and µ-Sb. The simple operation, remarkable improvement, and wide applications indicate the promising prospects of this strategy for advanced electrodes in sodium ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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Science Bulletin · 2024 · IF 18.8

Deciphering the potential of potassium-ion batteries beyond room temperature

Weihao Xia,Fengjun Ji,Yunzhuo Liu,Zhen Han,Kaikai Li,Jingyu Lu,Wei Zhai,Deping Li,Lijie Ci

Alloying-type anode materials are considered promising candidates for next-generation alkali-ion batteries. However, they face significant challenges owing to severe volume variations and sluggish kinetics, which hinder their practical applications. To address these issues, we propose a universal synthetic strategy, which can realize the facile synthesis of various alloying-type anode materials composed of a porous carbon matrix with uniformly embedded nanoparticles (Sb, Bi, or Sn). Besides, we construct the interactions among active materials, electrolyte compositions, and the resulting interface chemistries. This understanding assists in establishing balanced kinetics and stability. As a result, the fabricated battery cells based on the above strategy demonstrate high reversible capacity (515.6 mAh g −1 ), long cycle life (200 cycles), and excellent high-rate capability (at 5.0 C). Additionally, it shows improved thermal stability at 45 and 60 °C. Moreover, our alloying-type anodes exhibit significant potential for constructing a 450 Wh kg −1 battery system. This proposed strategy could boost the development of alloying-type anode materials, aligning with the future demands for low-cost, high stability, high safety, wide-temperature, and fast-charging battery systems.

研究领域: 材料科学 · 电化学 · 能源存储
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

In Situ Electrochemical Polymerization to Construct Robust Solid Electrolyte Interphase for Advanced Alloy-Type Anode Materials in Sodium-Ion Batteries

Chen Zhao,Cheng Zheng,Qian Yao,Chenghui Zhang,Jian Yang

High-quality solid electrolyte interphases (SEI) are important to advanced sodium-ion batteries, particularly on anode materials. Their large structure strain/stress usually aggravates the rupture and dissolution of the SEI, then degrades the electrochemical performance. Here, sodium vinylsulfonate (SVS) is reported as a model to achieve the polymer incorporation into the SEI by in situ electrochemical polymerization. The sulfonate group in SVS activates the vinyl group and interacts with the other components, enabling the polymer to be a robust and flexible backbone of the SEI. This enhances the mechanical properties and reduces the SEI dissolution, improving the electrochemical performance of anode materials. Using commercial tin microparticles (µ-Sn) as an example, they exhibit a capacity of 516.3 mAh g −1 after 2000 cycles at 4 A g −1 , a record-high performance at high rates. This strategy is also successful in the cases of µ-Bi and µ-Sb. These results are obtained based on commercial microparticles without carbon coating. So, it is believed that it is a new and simple way to improve the electrochemical performance of Na-ion batteries.

研究领域: 电化学 · 能量存储与转换 · 材料科学 · 电池技术
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