Nature Chemistry
·
2024
·Vol. 16
·期 3
·373-379
·
IF 19.2
Guan Yeqin,Wen Hong,Cui Kaixun,Wang Qianru,Gao Wenbo,Cai Yongli,Cheng Zibo,Pei Qijun,Li Zhao,Cao Hujun,He Teng,Guo Jianping,Chen Ping
Photon-driven chemical processes are usually mediated by oxides, nitrides and sulfides whose photo-conversion efficiency is limited by charge carrier recombination. Here we show that lithium hydride undergoes photolysis upon ultraviolet illumination to yield long-lived photon-generated electrons residing in hydrogen vacancies, known as F centres. We demonstrate that photon-driven dehydrogenation and dark rehydrogenation over lithium hydride can be fulfilled reversibly at room temperature, which is about 600 K lower than the corresponding thermal process. As light-driven F centre generation could provide an alternative approach to charge carrier separation to favour chemical transformations that are kinetically or thermodynamically challenging, we show that light-activated lithium hydride cleaves the N≡N triple bond to form a N–H bond under mild conditions. Co-feeding a N 2 /H 2 mixture with low H 2 partial pressure leads to photocatalytic ammonia formation at near ambient conditions. This work provides insights into the development of advanced materials and processes for light harvesting and conversion.
研究领域:
化学
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材料科学
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催化
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光化学
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高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yefei Wang,Fei Chang
The development of supported metal hydride catalysts with abundant active sites is a highly desirable yet challenging endeavor in ammonia synthesis. In this work, a lithium hydride (LiH)-loaded Fe/N-co-doped porous carbon (Fe-N-C) composite (LiH/Fe-N-C) was synthesized and demonstrated as an efficient catalyst for ammonia synthesis under mild conditions. The deposition of LiH onto Fe-N-C induced a partial reduction of the Fe-N moiety, resulting in the slight aggregation of isolated Fe single-atom sites into nanoparticles. Under reducing conditions (in the presence of H2), the coordinated nitrogen in Fe-N-C can be removed, forming nitrogen vacancies (VN), while surface iron hydride species (Fe-H) are generated through the interaction between LiH and Fe-N-C. The presence of Fe atoms adjacent to VN facilitates the adsorption and activation of dinitrogen, a process that is further supported by the replenishment of VN under reaction conditions. Notably, no lithium imide or amide species (Li2NH or LiNH2) — typically regarded as key intermediates in LiH-mediated ammonia synthesis, were observed on LiH/Fe-N-C, likely due to the fast hydrogenation step. Consequently, LiH/Fe-N-C achieves an ammonia production rate of 872 mmol·gFe-1·h-1, surpassing the performance of state-of-the-art Fe-based catalysts at 300 oC and 1 MPa. This study demonstrates that the synergistic catalysis of LiH, transition metals, and their adjacent nitrogen vacancies offers a promising pathway for efficient ammonia synthesis under mild conditions.
研究领域:
催化化学
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材料科学
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可持续能源
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无机化学
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高影响因子
Journal of Energy Storage
·
2026
·
IF 9.8
Tangqi Hu,Wen Huang,Wei Liu,Yonggang Yang,Yi Li
The self-assembled ordered structure of liquid crystal polymer networks (LCNs) can construct specific channels through the LC molecular orientation, benefitting the ordered transport of Li ions. Meanwhile, single-ion conducting polymer electrolytes can effectively enhance the safety of lithium-ion batteries by raising the lithium transference number ( t Li + ) and preventing the growth of lithium dendrites. Herein, Li salt grafted nematic LCN was coated on poly(vinylidene fluoride-hexafluoropropylene) (P(VDF-HFP)) membrane to make NLCN-Li/Pv and NLCN-Li/Pv/N composite membranes according to the single- or double-sided way. After coupling with plasticizer, quasi-solid-state electrolyte membranes have been successfully produced. The electrochemical tests disclosed that they possessed benign thermal stability and electrolyte/electrode compatibility. The high t Li + over 0.7 indicated their near single-ion conductive characteristic. A small amount (0.5 M) of extra Li salt added to the plasticizer could effectively improve the ion conductivity ( σ ) while the t Li + remained around 0.7. Moreover, the doping of silica nanoparticles into the NLCN-Li layer furtherly increased the σ up to 1.5 × 10 −4 S cm −1 while the t Li + rose to 0.88. The assembled LFP|Li cells also showed outstanding cycling stability and rate capabilities, indicating the applicability of the composite electrolyte membrane and providing insights into the design and preparation of ordered quasi-solid-state electrolytes for high-performance and safe secondary batteries.
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CERAMICS INTERNATIONAL
·
2026
·
IF 6
Biao Yi,Guangfan Tan,Yanwei Huang,Dajun Xu,Yingjie Guo,Yingchun Zhang
Lithium hydride (LiH) is a neutron shielding material for space nuclear reactors, but research on its preparation, processing, and functional integration remains limited. This study systematically investigates the preparation process and properties of LiH ceramics to evaluate their potential application in neutron shielding systems for space reactors. Green bodies were prepared via cold pressing and sintered at 500°C, yielding highly dense (98%) ceramics with closed pores, uniformly distributed grains (3–5 μm), stable microstructure, and no significant cracks. Mechanical testing revealed compressive strength reaching 180.67 MPa and flexural strength of 35.21 MPa at the optimal sintering temperature. Thermal performance tests indicated that the ceramic's thermal conductivity exceeded that of the green body and exhibited a decreasing trend across a broad temperature range from room temperature to 500°C, demonstrating stable and predictable thermal behavior. Both MCNP simulations and experimental measurements using a 252 Cf neutron source confirm that thin-layer LiH ceramics achieve over 90% shielding efficiency for low to medium energy neutrons and demonstrate significant shielding effects for fast neutrons. Comprehensive analysis indicates that LiH ceramics can simultaneously achieve high density, excellent mechanical and thermal properties, and outstanding neutron shielding capability. This provides reliable process guidance for the design and application of shielding materials.
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MOLECULES
·
2026
·Vol. 31
·期 16
·2879
·
IF 5.1
Tangqi Hu,Junxian Fu,Yonggang Yang,Yi Li
Self-assembled liquid crystal polymer networks build directional transport channels via molecular alignment, enabling efficient and ordered lithium-ion migration, while single-ion conducting polymer electrolytes improve lithium-ion transference number by covalently anchoring anions, which alleviates concentration polarization and effectively suppresses lithium dendrite growth. Herein, a series of substrate-free Li salt-grafted cholesteric liquid crystal elastomers (CLCE) with tunable helical pitches and spiral orientation were fabricated, and quasi-solid electrolyte membranes were obtained through plasticization. It was found that samples with the smallest helical pitch delivered the highest lithium-ion transference number irrespective of the spiral orientation. The optimal CLCE electrolyte membrane achieved a lithium-ion transference number of 0.94, exhibiting characteristic single-ion conductivity. Moreover, after adding small amount of extra free Li salt, the prepared electrolyte membrane delivered a room-temperature ionic conductivity of 2.6 × 10−4S·cm−1, an electrochemical stability window of 5.2 V and stable cycling performance, providing new insights into the design of high-performance safe quasi-solid lithium-ion batteries.
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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Qiongyu Wang,Ziheng Zhang,Xilun Zhang,Hua Xie,Ling Jiang,Fei Chang
Catalytic alkyne semi-hydrogenation is a pivotal industrial transformation currently constrained by the limitations of existing heterogeneous catalysts: precious metals (e.g., Pd) face high costs, while non-precious alternatives (e.g., Ni, Cu, Fe) generally require harsh reaction conditions (100–200 °C, 10–40 bar H 2 ). To address these persistent challenges, we propose a novel strategy integrating alkali metal hydrides, serving simultaneously as hydrogen donors and anionic “ligands” into transition metal systems. Herein, we report a NiFe-LiH composite catalyst that enables efficient and highly selective liquid-phase semi-hydrogenation of alkynes—including aliphatic, aromatic, and heteroatom-substituted substrates under very mild conditions (25 °C, ≤3 bar H 2 ). Mechanistic investigations reveal that reactive hydride species (H − ) are integral to the hydrogenation catalysis. Critically, the formation of unique Li-Ni-Fe-H interfacial species facilitate synergistic interactions wherein anionic hydrides coordinate with transition metals, modulating their electronic states to simultaneously enhance catalytic activity and selectivity. This work demonstrates room-temperature activation and transformation of alkynes enabled by a catalytic Li-Ni-Fe-H system, offering a promising new pathway for developing efficient non-noble metal catalysts for selective hydrogenation reactions.
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RARE METALS
·
2025
·
IF 11
Liu Yu-Kun,Pang Yu-Chen,Li Chao-Qun,Zhang Xiao-Yue,Hu Xue-Chun,Chen Wei,Yu Xue-Bin,Xia Guang-Lin
As a typical reactive composite hydrogen storage system, 2LiBH 4 –MgH 2 holds an ultrahigh hydrogen storage capacity of 11.5 wt%. However, it suffers from sluggish hydrogen storage kinetics due to the difficult nucleation of MgB 2 . Herein, amorphous VB 2 nanoparticles with an average size of approximately 32 nm are synthesized to enhance the hydrogen storage performance of 2LiBH 4 –MgH 2 composite. VB 2 , sharing the same hexagonal structure with MgB 2 with a d -value mismatch ratio of only 2.28%, could serve as effective nucleation sites for promoting the formation of MgB 2 . Theoretical calculations reveal that the introduction of VB 2 significantly reduces the binding energies of B and Mg, facilitating in situ nucleation of MgB 2 . As a result, after the introduction of VB 2 nanoparticles, complete hydrogen desorption of 9.23 wt% is achieved for 2LiBH 4 -MgH 2 within 2 h at 400 °C, which is 4 times shorter than the time required for pure 2LiBH 4 -MgH 2 , and no nucleation incubation period for hydrogen desorption is observed even at a low temperature of 380 °C. More importantly, a reversible capacity of 9.3 wt%, corresponding to a capacity retention of 100%, could be preserved after 10 cycles of hydrogen storage, demonstrating stable reversible hydrogen storage performance. This study provides a novel technological pathway for improving the reversible hydrogen storage performance of composite metal hydrides and offers significant insights into the development of high-performance hydrogen storage materials. Graphical
研究领域:
材料科学
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能源存储
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RSC Advances
·
2025
·Vol. 15
·期 44
·37273-37287
·
IF 4.6
Ya Gao,Haoping Huo,Jianlin Li,Nengqing Wang,Haonan Gao,Yingbo Wang
Eradicating cutaneous infections induced by pathogenic microorganisms, such as bacteria, fungi, and viruses, via conventional topical drug delivery is challenging owing to limited epidermal penetration. To overcome this limitation, we fabricated a poly(ethylene glycol) diacrylate (PEGDA) microneedle array coated with a carboxymethyl chitosan (CMC) film embedded within situ-synthesized polydopamine-modified silver nanoparticles (PDA@Ag NPs) for enhanced antibacterial efficacy. This design utilizes microneedle (MN)-mediated skin perforation to enhance drug permeation, combined with rapid film dissolution for the efficient release of the payload. The experimental findings revealed that the PDA@Ag-CMC/PEGDA MNs possess favorable biocompatibility along with dual photothermal and photodynamic functionalities. Mild photothermal therapy (PTT) triggered by these MNs promotes the production of antibacterial reactive oxygen species (ROS), resulting in a high antibacterial rate of up to 98% against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) under NIR irradiation at a PDA@Ag concentration of 40 μg mL−1. To assess transdermal delivery performance, lidocaine hydrochloride (LiH) (78 μg per MN array) was incorporated into the CMC film as a model drug. Physiological conditions confirmed accelerated LiH release from the PDA@Ag-LiH-CMC/PEGDA system upon aqueous exposure. This minimally invasive approach demonstrated promising broad-spectrum antibacterial activity, suggesting that the PDA@Ag-LiH-CMC/PEGDA platform could serve as a viable clinical solution for managing polymicrobial skin infections and alleviating wound pain.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Zhiqiang Dai,Xueqing Zhang,Kittima Lolupiman,Chengwu Yang,Pattaraporn Woottapanit,Wanwisa Limphirat,Suttipong Wannapaiboon,Xinyu Zhang,Jiaqian Qin
The limited availability of cathode materials for rechargeable aqueous zinc-ion batteries (ZIBs), which have great potential for grid-scale energy storage applications, remains a significant obstacle to development. In this study, we proposed a Li3VO4–LiV2O5-based (LiVO-w) nanocomposite structure obtained by simple high-temperature calcination and water washing as a high-performance cathode. The LiVO-w cathode demonstrates a high specific capacity (310.43 mAh g–1 at 1 A g–1 and 130.52 mAh g–1 at 20 A g–1) and excellent cycling stability (100% capacity retention after 4000 cycles at 10 A g–1 and 85.13% capacity retention after 10,000 cycles). In addition, ex situ X-ray diffraction (XRD) shows the structural transformation of LiVO-w during the self-assembly process. During the first charge process, the multivalent and multistructured LiVO-w undergoes an increase in the valence of V, accompanied by the generation of Zn3(OH)2V2O7·H2O on the surface of the matrix. The charge and discharge process after self-assembly mainly corresponds to the generation and decomposition of Zn3(OH)2V2O7·H2O. This excellent self-assembled matrix realizes the realization of LiVO-w cathodes with high capacity and high-capacity retention, representing a major advancement in the commercial development of ZIBs for the development of LiVO-w positive electrode materials.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Guoquan Na,Wen-Gang Cui,Hangyan Shi,Zhenglong Li,Fan Gao,Yong Gao,Xingqiang Wang,Ke Wang,Yaxiong Yang,Zichao Shen,Yanxia Liu,Hongge Pan
Lithium borohydride (LiBH 4 ) is a promising high-density hydrogen storage material, but its practical application is hindered by high dehydrogenation temperatures, slow kinetics, and poor stability. Catalytic modification is an effective strategy to overcome these limitations. In this work, a LiBH 4 -based composite co-modified with 20 wt% Ni and 10 wt% BN (denoted as LiBH 4 @20Ni10BN) was synthesized via one-step ball milling. The LiBH 4 @20Ni10BN begins to dehydrogenate at 230 °C and releases 7.1 wt% H 2 at 350 °C. Moreover, it rapidly desorbs 4.9 wt% H 2 within 60 min at 320 °C. The performance improvement is attributed to the synergistic catalysis of Ni and BN, where BN weakens the B–H bonds and Ni in situ transforms into the highly active NiB 2 during the first dehydrogenation. The stable BN and newly formed NiB 2 collectively contribute to superior cycling stability, maintaining a reversible capacity of 4.0 wt% after eight cycles.
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NATURE
·
2025
·Vol. 646
·期 8083
·102-107
·
IF 48.5
Liu Xiangsi,Li Shuyang,Yuan Chen,Zheng Bizhu,Cheng Gangya,Chen Yufan,Lu Xingyu,Gu Danyu,Lv Baijiang,Li Hao,Yan Zihan,Qian Hui,Zhu Yizhou,Sun Dalin,Song Yun,Xiang Yuxuan
The electrolyte–electrode interface serves as the foundation for a myriad of chemical and physical processes. In battery chemistry, the formation of a well-known solid–electrolyte interphase (SEI) plays a pivotal role in ensuring the reversible operations of rechargeable lithium-ion batteries (LIBs) 1 , 2 . However, characterizing the precise chemical composition of the low crystallinity and highly sensitive SEI presents a formidable challenge 3 . Here, taking lithium fluoride (LiF)—a widely studied and considered crucial SEI component 4 , 5 , 6 , 7 —as an example, we use 19 F solid-state nuclear magnetic resonance (NMR) and identify that LiF formed in SEI (LiF SEI ) has fruitful spectroscopy features that originated from the formation of limited LiF–LiH solid solutions: H-rich phase (LiH 1 − y F y ) and F-rich phase (LiF 1 − x H x ), which is further validated by 6 Li isotope NMR, synchrotron X-ray diffraction and cryo-electron microscopy (cryo-EM). By characterizing SEI formed in various electrolytes, we confirm the dominance of LiH 1 − y F y in high-coulombic-efficiency electrolyte, which can be rationalized by the fact that LiF–LiH solid solution shows improved ionic conductivity over LiF. As a proof of concept, we demonstrate that LiH 1− y F y -rich coating layer presents obvious advantages compared with LiF-rich coating layer in lithium-metal batteries. This revised understanding of the heterogeneous nature of SEI components would provide new insights for electrode–electrolyte interface design.
研究领域:
电化学
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材料科学
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能源化学
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固体化学
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电池技术
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Hui Peng,Tangqi Hu,Wen Huang,Wei Liu,Yonggang Yang,Yi Li
Single-ion conductive polymer electrolytes can effectively enhance the safety of lithium ion batteries (LIBs) by increasing the lithium transference number ( t Li + ) and avoiding the growth of lithium dendrites. Meanwhile, self-assembled ordered structure of liquid crystal polymer networks (LCNs) can form specific channels via the LC molecular orientation, benefiting the ordered transport of Li ions. Herein, two single-ion conductive smectic LCN electrolyte membranes coated on poly(vinylidene fluoride-hexafluoropropylene) (P(VDF-HFP)) film (denoted as SLCN-Li/Pv) were prepared by different ways. For comparison, one disordered polymer network electrolyte membrane coated on P(VDF-HFP) (denoted as DPN-Li/Pv) was also prepared. After coupling with plasticizer, three quasi-solid-state electrolyte membranes have been successfully produced. Their electrochemical properties were evaluated, and it was found that they possessed benign thermal stability and electrolyte/electrode compatibility. The high t Li + of 0.87 for SLCN-Li/Pv indicated their near-single-ion conductive characteristic. A small amount (0.5 M) of extra Li salt adding to the plasticizer could effectively improve the ion conductivity from 5.58 × 10 −6 to 1.58 × 10 −5 S cm −1 , while the t Li + remained 0.77. The assembled LFP|Li batteries also exhibited excellent cycling and rate performances. Compared with DPN-Li/Pv, SLCN-Li/Pv exhibited higher σ and t Li + , indicating that the orderliness of LC molecular orientation played an important role in the distribution and moving of Li ions, thereby affected the Li deposition and growth of Li dendrites. As the first report of smectic LCN single-ion conductors, this work throws light on the design and fabrication of ordered quasi-solid-state electrolytes for high-performance and safe LIBs.
研究领域:
材料科学
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电化学
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储能技术
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高分子科学
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锂离子电池
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