CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 45
·10314-10320
·
IF 4.857
Guiqiang Cao,Zhikang Wang,Da Bi,Jing Zheng,Qingxue Lai,Yanyu Liang
Graphical Atomic cat : A single-atom Fe@NG electrocatalyst serves as the coating of separators for high-performance Li-S batteries. Atomically dispersed Fe sites on the graphene framework promote the conversion efficiency of LiPS. The Fe@NG electrocatalyst delivers an initial capacity of 1616 mA h g −1 at 0.1 C, and a reversible capacity of 546 mA h g −1 after 200 cycles at 2 C (70 % capacity retention). Lithium-sulfur batteries have been considered as potential electrochemical energy-storage devices owing to their satisfactory theoretical energy density. Nonetheless, the inferior conversion efficiency of polysulfides in essence leads to fast capacity decay during the discharge/charge cycle. In this work, it is successfully demonstrated that the conversion efficiency of lithium polysulfides is remarkably enhanced by employing a well-distributed atomic-scale Fe-based catalyst immobilized on nitrogen-doped graphene (Fe@NG) as a coating of separator in lithium-sulfur batteries. The quantitative electrocatalytic efficiency of the conversion of lithium polysulfides is determined through cyclic voltammetry. It is also proven that the Fe-N X configuration with highly catalytic activity is quite beneficial for the conversion of lithium polysulfides. In addition, the adsorption and permeation experiments distinctly indicate that the strong anchoring effect, originated from the charge redistribution of N doping into the graphene matrix, inhibits the movement of lithium polysulfides. Thanks to these advantages, if the as-prepared Fe@NG catalyst is combined with polypropylene and applied as a separator (Fe@NG/PP) in Li-S batteries, a high initial capacity (1616 mA h g −1 at 0.1 C), excellent capacity retention (93 % at 0.2 C, 70 % at 2 C), and superb rate performance (820 mA h g −1 at 2 C) are achieved.
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高影响因子
RSC Advances
·
2025
·Vol. 15
·期 56
·48487-48497
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IF 4.6
Yong Liu,Bohon Chen,Hanbin Nie,Shuanglin Gui,Jianping Deng
Electrolytic hydrogen production from water is a cost-effective renewable energy technology, but its development is severely constrained by high energy consumption, precious metal catalysts, and low-value products of anode. Given that inexpensive glycerol exhibits a significantly lower redox potential than water, this study developed a 3D coral-like nickel–molybdenum sulfur bifunctional nanocatalyst (Ni–Mo–S/NF) based on nickel foam, which served as both the anode and cathode in an alkaline glycerol electrolyte, enabling the simultaneous production of high-value formate at the anode and high-purity hydrogen at the cathode. Notably, in a two-electrode system, the alkaline glycerol electrolyzer required only 1.37 V to achieve a current density of 10 mA cm−2, which was 280 mV lower than that of an alkaline aqueous solution system, indicating an about 17% reduction in energy consumption compared to conventional water electrolysis. Meanwhile, this system reached a faradaic efficiency of 95.0% for formate production and 99.6% for hydrogen evolution. Benefiting from the outstanding performance of the noble-metal-free Ni–Mo–S/NF catalyst, the proposed technology for simultaneous formate and hydrogen production via glycerol electrooxidation offers a novel pathway for the green production of high-value chemicals and energy-saving hydrogen generation.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Hongxing Wang,Zhipeng Yin,Chengwei Ma,Zipeng Sun,Hao Feng,Fei Chen,Jiangqi Zhou,Tinglu Song
Lithium–sulfur (Li–S) battery systems are universally recognized as frontrunners in next-generation energy storage owing to their energy densities exceeding 2600 Wh kg–1. Nevertheless, their practical implementation remains constrained by severe Li metal anode degradation caused by polysulfide shuttle mediated corrosion, which drastically decreases achievable energy densities. This work pioneers an innovative interfacial engineering strategy leveraging transition metal ion synergies to fundamentally address this challenge. Through chemically induced anion modulation, nickel species spontaneously reconfigure into a protective solid electrolyte interphase (SEI) at Li surfaces. This engineered inorganic-dominant architecture demonstrates dual functionality that effectively passivates polysulfide-induced electrochemical corrosion and dramatically curtails electrolyte decomposition kinetics. Remarkably, even in LiNO3-free configurations, the optimized system achieves exceptional cycling stability (76.4% capacity retention). These findings establish a paradigm-shifting framework for developing practically viable high energy density Li–S systems through a rational interface design.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Wutao Wei,Xi Jia,Xuyan Qin,Zhikai Wang,Yide Zhang,Fang He,Liwei Mi
Magnesium/lithium-sulfur hybrid batteries (ML-SHBs) are considered to be the strongest candidate to replace lithium-ion batteries (LIBs) due to their high volumetric energy density and dendrite-free. In this study, S@FeS 2 /CoS 2 was prepared on the basis of a hollow, eggshell-shaped construction by using the less-liquid method. In this method, the reactants carry water of crystallization during the reaction to provide a liquid environment, and the metal ions on the surface of the droplets promote the formation of S@FeS 2 /CoS 2 . The configuration of the eggshell facilitates the generation of additional reaction interfaces, thereby expediting the interaction with the electrolyte and facilitating transport processes. This structure promotes efficient charge transfer and accelerates the transport rate. By implementing strategies such as heterostructure building and bimetallic doping, the controllable construction of the morphological structure can be realized. The induced effect of heterostructured interfaces can be excited within the nanocrystals to form an electric field, which effectively reduces the ion diffusion barrier and synchronously enhances the interfacial electron transfer efficiency by modulating the electronic behavior. The discharge specific capacity of the cell was found to be 1096.73 mAh g −1 at a current density of 200 mA g −1 , exhibiting a high rate capacity. The Coulombic efficiency remained at 99.8 % after 100 cycles at a current density of 500 mA g −1 .
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JOURNAL OF TRACE ELEMENTS IN MEDICINE AND BIOLOGY
·
2022
·
IF 3.995
Chunliang Liu,Zerong Wang,Wei Wang,Lei Zheng,Ming Li
Background It is a consensus that selenomethionine (SeMet) can protect liver from damage, but the immune mechanism of SeMet in acute liver injury (ALI) is still unclear. This study aims to investigate the protective effects of SeMet against ALI and to elucidate the possible immune mechanism. Methods Firstly, the role of SeMet in CCl 4 -induced ALI mice was investigated through survival rate, serum ALT and AST, liver necrosis and apoptosis analysis. The expression and secretion of inflammatory cytokines and chemokines in the liver and serum of CCl 4 -induced ALI mice were analyzed by qRT-PCR and ELISA. Then the immune cell phenotypes were analyzed by flow cytometry and confocal imaging. In addition, MDSCs depletion, CXCL12/CXCR4 axis blocking and selenoprotein S (SELENOS) knockdown assays were used to reveal the immune mechanism of SeMet. Results We found that SeMet prolonged survival rate, decreased the serum ALT and AST, alleviated liver necrosis and inhibited hepatocytes apoptosis. Prospective, SeMet decreased the expression of IL-6 and TNF-α, and increased the expression of IL-10. Interestingly, SeMet decreased the expression of MCP-1, while increased the expression of CXCL12. The immune analysis showed that SeMet decreased the activation of T cells through promoting MDSCs accumulation mediated by CXCL12/CXCR4 axis. Furthermore, SeMet increased SELENOS expression in vivo , and knockdown of SELENOS effectively abolished the protective effect of SeMet during ALI. Conclusion This study demonstrates that SeMet alleviates CCl4-induced ALI by promoting MDSCs accumulation through SELENOS mediated CXCL12/CXCR4 axis. Therefore, our study infers that selenium intake may be as a new therapeutic option for management of inflammation-mediated liver injury.
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CEMENT AND CONCRETE RESEARCH
·
2025
·
IF 13.1
Xin Liu,Dining Li,Hui Xie,Jiachen Yao,Xuyan Shen,Haochuan Wang,Zhengyao Qu,Zuhua Zhang,Pan Feng
Alkali-free aluminum sulfate (AS)-based accelerators have become a widely adopted and indispensable admixture for shotcrete applications. However, their effects on the formation kinetics and properties of calcium silicate hydrate (C-S-H) – the primary hydrate in shotcrete – remain insufficiently understood. To bridge this knowledge gap, a combination of isothermal calorimetry, QXRD, and TGA was employed to uncover the temporal evolution of C-S-H. In addition, the chemical compositions and silicate chain structure were comprehensively examined using BSE-EDS, 27 Al NMR, coupled with 29 Si NMR techniques. Our results demonstrate that AS addition accelerated C 3 S hydration, promoting the C-S-H nucleation and growth rate. This acceleration effect can be ascribed to (1) the accelerated dissolution of silicate phases at early stages, and (2) the formation of divergent C-S-H needles, providing more nucleation sites while mitigating impingement between adjacent C-(A)-S-H needles. Multiple characterizations confirmed the enhanced incorporation of aluminum into C-S-H, predominately at the bridging site. Notably, increasing AS content decreased the Si/Ca of the C-(A)-S-H and concurrently enhanced the aluminum incorporation. This compositional shift led to the formation of longer aluminosilicate chains and concomitant improvements in the hardness and elastic modulus of C-(A)-S-H. These findings offer valuable insights into AS-induced alterations in C-(A)-S-H within accelerated cement pastes, facilitating the deeper understanding of the role of C-(A)-S-H in strength development and long-term durability of shotcrete.
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Small
·
2018
·Vol. 14
·期 41
·1802443
·
IF 9.598
Xiao-Tian Gao,Ying Xie,Xiao-Dong Zhu,Ke-Ning Sun,Xu-Ming Xie,Yi-Tao Liu,Jian-Yong Yu,Bin Ding
Being conductive and flexible, 2D transition metal nitrides and carbides (MXenes) can serve in Li–S batteries as sulfur hosts to increase the conductivity and alleviate the volume expansion. However, the surface functional groups, such as OH and F, weaken the ability of bare MXenes in the chemisorption of polysulfides. Besides, they create numerous hydrogen bonds which make MXenes liable to restack, resulting in substantial loss of active area and, thus, inaccessibility of ions and electrolyte. Herein, a facile, one-step strategy is developed for the growth of TiO 2 quantum dots (QDs) on ultrathin MXene (Ti 3 C 2 T x ) nanosheets by cetyltrimethylammonium bromide-assisted solvothermal synthesis. These QDs act as spacers to isolate the MXene nanosheets from restacking, and preserve their 2D geometry which guarantees larger electrode–electrolyte contact area and higher sulfur loading. The stronger adsorption energy of polysulfides with TiO 2 (than with Ti 3 C 2 T x ), as proven by density functional theory calculations, is essential for better on-site polysulfide retention. The ultrathin nature and protected conductivity ensure rapid ion and electron diffusion, and the excellent flexibility maintains high mechanical integrity. In result, the TiO 2 QDs@MXene/S cathode exhibits significantly improved long-term cyclability and rate capability, disclosing a new opportunity toward fast and stable Li–S batteries.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Di Wu,Wen Ren,Yang Yang,Jiulin Wang,Yanna NuLi
A magnesium–sulfur (Mg–S) battery system is considered a high-performance candidate for next-generation secondary batteries, because of its prominent advantages such as high safety, low cost, and high energy density. However, the shuttle effect caused by the dissolution of polysulfides leads to irreversible loss of capacity. Herein, we prepare a S0.96Se0.04@CMK3 composite (with a high S + Se content of 82.6 wt %) and employ the composite material as a cathode for Mg batteries with easily prepared hybrid electrolytes. The electronic conductivity of the cathode material increases by 18 orders of magnitude after Se doping, from 5 × 10–28 to 6.5 × 10–10 S m–1. Compared with S@CMK3, doped Se in S0.96Se0.04@CMK3 plays an important role in maintaining capacity stability by lowering polarization, facilitating electron transport, and improving reaction kinetics. The S0.96Se0.04@CMK3 cathode delivers a stable and reversible capacity of 492.9 mAh g–1 after 110 cycles, which is almost twice that of the S@CMK cathode without Se doping, and better rate performance. This Se-doping strategy proposes an effective method to exploit high-performance cathodes for Mg–S batteries.
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JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Bohong Chen,Zhongqing Jiang,Lingshan Zhou,Binglu Deng,Zhong-Jie Jiang,Jianlin Huang,Meilin Liu
A simple synthetic method is developed for the synthesis of CoS 2 /N, S-codoped graphene. The result shows the existence of a strong electronic coupling between CoS 2 and N, S-codoped graphene. The pyrrolic and pyridinic type nitrogen and S in the form of C-S-C in N, S-codoped graphene are found to be the anchoring sites of the CoS 2 nanoparticles . As a bifunctional catalyst , the CoS 2 /N, S-codoped graphene exhibits an oxygen reduction onset potential of 0.963 V vs. RHE and delivers an oxygen evolution overpotential of 393 mV at the current density of 10 mA cm −2 . Its oxygen reduction and evolution catalytic activities are comparable to those of the Pt/C and the state-of-art RuO 2 /C, respectively. Most impressively, the CoS 2 /N, S-codoped graphene exhibits a potential gap of 771 mV. This value is lower than those of most bifuntional catalysts reported, clearly indicating its potential use as the bifunctional catalyst to replace the noble-metal based catalysts for practical applications. Additionally, our results also suggest a great importance to prepare a single pure phase CoS 2 in improving the catalytic bifunctionality of the CoS 2 /N, S-codoped graphene. The primary Zn-air battery with CoS 2 /N, S-codoped graphene shows a higher discharge peak power density than that with Pt/C.
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Journal of the American Chemical Society
·
2019
·
IF 14.695
Ruijin Sun,Shifeng Jin,Lin Gu,Qinghua Zhang,Qingzhen Huang,Tianping Ying,YiRan Peng,Jun Deng,Zhiping Yin,Xiaolong Chen
The pairing of ions of opposite charge is a central principle of chemistry. Even though the ability to intercalate anions is desirable for many applications, it remains a key challenge for numerous host materials with their outmost layers beingn anions. In this work, we introduce a hydrothermal ion-exchange synthesis to intercalate oxidative S and Se anions between the Se layers of FeSe, which leads to single crystals of novel compounds (Se/S)x(NH3)yFe2Se2. In particular, the unusual anion–anion bonding between the intercalated S (or Se) and Se layers exhibits strong ionic characteristics. The charge transfer through the Se layer to S (or Se) intercalants is further confirmed by the elevated oxidation state of Fe ions and the dominant hole carriers in the intercalated compounds. By intercalating S, for the first time superconductivity emerged in hole-doped iron chalcogenides. The generality of this chemical approach was further demonstrated with layered FeS and NiSe. Our findings thus open an avenue to exploring diverse aspects of anionic intercalation in similar materials.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Cong Liu,Fenyun Yi,Dong Shu,Weixin Chen,Xiaoping Zhou,Zhenhua Zhu,Ronghua Zeng,Aimei Gao,Chun He,Xia Li
Three-dimensional N/S co-doped succulent-like hierarchical carbon (3D NS-SHC) is synthesized by carbonization of a supramolecular cluster. In this supramolecular process, potassium citrate can act as a reliable carbon source, while the thiourea as a N/S source and then, two molecules gradually tend to generate a giant “all-in-one” precursor via hydrogen bonding verified by Independent Gradient Model (IGM) calculation. TEM and SEM images show the N/S co-doped carbon holds a novel 3D succulent-like hierarchical structure. For NS-SHC-8:8 sample, element mapping images display the uniform N/S atoms distribution. These distinct features can be related to the supramolecular polymerization which promotes in-situ N/S co-doping homogenously and conduces to build 3D structure. Typically, NS-SHC-8:8 electrode exhibits prominent specific capacitance (258.5 F g −1 at 0.5 A g −1 ) and excellent cycle stability (94.4% after 20000 cycles) in three-electrode system. Furthermore, an assembled quasi-solid state symmetric supercapacitor delivers good energy density (10.2 Wh kg −1 at 250 W kg −1 ) and steady cycle endurance (85.1% after 10000 cycles). These eximious behaviors of NS-SHC-8:8 are mainly attributed to (1) the uniform N/S atoms distribution and their synergistic effect, which brings extra Faradaic reaction to higher specific capacitance, (2) the charming 3D succulent-like hierarchical structure, which serves as a multifunctional reservoir that can accommodate the ion/charge and facilitate their migration to further promote the electrochemical performance. Above mentions suggest that this uniformly heteroatom-modified carbon material produced by supramolecular technique is promising for high-performance energy storage devices.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 39
·22684-22690
·
IF 12.732
Di Yu,Qian Zhang,Jie Liu,Ziyang Guo,Lei Wang
High-loading sulfur electrodes play a crucial role in the practical application of Li–S batteries. However, the poor mechanical stability and sluggish Li-ion conduction severely hinder the cycling stability and rate property of high-loading sulfur electrodes. PVDF binder has been widely used in Li–S batteries, while the coating process using PVDF binder requires toxic and expensive NMP solvent and the poor mechanical property of PVDF binder makes it incompetent as the binder for high-loading Li–S batteries. Herein, we use strong-affinity alginic acid (Alg) and high-wettability, high-modulus isosorbide (IS) to produce an environmentally friendly c-Alg-IS network binder via a condensation reaction for a high-loading sulfur electrode. As a result, a Li–S battery with a c-Alg-IS binder showed dramatically improved cycling stability and rate performance under high sulfur loading; especially, when the sulfur loading increases to 9.1 mg cm−2, the Li–S battery exhibits a stable cycling life of 60 cycles and high areal capacity of 7.2 mA h cm−2 at 2.4 mA cm−2. This work provides a simple and effective strategy to address the issues of poor cycling stability and rate property of high-loading Li–S batteries.
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