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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Noble-metal-free Zn0.5Cd0.5S@MoS2 core@shell heterostructures for visible-light-driven H2 evolution with enhanced efficiency and stability

Xing-Liang Yin,Lei-Lei Li,Jian-Hua Jiang,Xin-Xin Du,Dong-Hui Pang,Jie Yang,Zhong-Jia Li,Yuan-Xu Wang,Xin-Yue Li,Da-Cheng Li,Jian-Min Dou

Photocatalytic H 2 evolution from water splitting offers an attractive scientific and technological method to address the energy and environmental crisis. In this study, noble-metal-free Zn 0.5 Cd 0.5 S@MoS 2 core@shell nanoheterostructures were elaborately designed and successfully synthesized. The visible-light-driven photocatalytic performance investigation shows that the Zn 0.5 Cd 0.5 S@MoS 2 exhibits a state-of-the-art H 2 evolution rate of 40.2 mmol g −1  h −1 far exceeding that of pristine Zn 0.5 Cd 0.5 S by more than 57 times. Moreover, thanks to the protection of MoS 2 shells, the Zn 0.5 Cd 0.5 S@MoS 2 can retain long-term stability in four-cycles of 24 h reactions. Furthermore, a tentative mechanism on H 2 generation was systematically investigated and proposed, which contributes to understand the enhanced photocatalytic activity of the Zn 0.5 Cd 0.5 S@MoS 2 heterostructures and may inspire the synthesis of other desirable catalytic systems.

研究领域: 材料科学 · 物理化学 · 能源化学 · 纳米催化 · 光化学
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Journal of Energy Chemistry · 2022 · IF 13.599

Engineering Pt heterogeneous catalysts for accelerated liquid–solid redox conversion in Li-S batteries

Qinhua Gu,Yujie Qi,Wuxing Hua,Tongxin Shang,Junnan Chen,Luozhen Jiang,Lina Li,Ming Lu,Yixiao Zhang,Xi Liu,Ying Wan,Bingsen Zhang

The shuttle effect caused by soluble lithium polysulfides (LiPSs) deteriorates multiphase transformation reaction kinetics of sulfur species, and gives rise to an unserviceable lithium-sulfur (Li-S) battery. Catalysis, as a process optimization approach, offers an option to eliminate the intrinsic issues. However, exploring and understanding the role of catalysts on electrode reaction remains critical bottlenecks, particularly as they are prone to continuous evolution under complex dynamic environment. Herein, platinum nanoparticles loaded on MXene nanosheets, as sulfur host, and the action of catalysts on the reaction process are investigated via ex-situ monitors upon solid–liquid–solid chemical transformation of sulfur species. These traces confirm that the high performance originates from electron transfer between catalysts and LiPSs, which lowers the nucleation barrier from liquid LiPSs to solid Li 2 S/Li 2 S 2 . Further, the accelerated liquid–solid conversion can alleviate the accumulation of LiPSs, and boost the reaction kinetics in Li-S batteries. The findings corroborate the electronic modulation between catalysts and LiPSs, which is a generalizable strategy to optimize energy conversion efficiency of Li-S batteries.

研究领域: 电化学 · 能源材料 · 纳米催化 · 电池化学 · 表面科学
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Journal of Energy Chemistry · 2020 · IF 7.216

A Li-S battery with ultrahigh cycling stability and enhanced rate capability based on novel ZnO yolk-shell sulfur host

Ruihan Zhang,Maochun Wu,Xinzhuang Fan,Haoran Jiang,Tianshou Zhao

Currently, lithium-sulfur (Li-S) batteries still suffer from fast capacity decay, poor coulombic efficiency (CE) and short cycling lifespan, which result from the severe shuttle effect issue caused by high solubility and rapid diffusion of lithium polysulfides (LiPSs) in organic electrolytes. Here, yolk-shell zinc oxide (YS-ZnO) spheres are synthesized and for the first time, applied as a host for Li-S batteries to tackle this challenge. The polar ZnO exhibits high chemical anchoring ability toward LiPSs while the unique yolk-shell structure not only provides an additional physical barrier to LiPSs but also enables much more uniform sulfur distribution, thus significantly suppressing LiPSs shuttling effect meanwhile promoting sulfur conversion reactions. As a result, the YS-ZnO enables the Li-S battery to display an initial specific capacity of 1355 mAh g −1 and an outstanding capacity retention capability (~89.44% retention rate) even after 500 cycles with the average CE of ~99.46% at the current of 0.5 C. By contrast, the capacity of conventional-ZnO-nanoparticles based battery severely decays to 472 mAh g −1 after cycling for 500 times. More impressively, the S/YS-ZnO based Li-S battery can maintain a low decay rate of 0.040% every cycle and high average CE of 98.82% over 1000 cycles at 3 C.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 电池技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

Entrapment of polysulfides by a Ketjen Black & mesoporous TiO2 modified glass fiber separator for high performance lithium-sulfur batteries

Lin Shan,Cai Yurong,Yang Jing,Ruan Feixia,Wu Jun,Sireesh Babu,Yao Xin,Gao Junkuo,Yao Juming

The application of lithium-sulfur batteries is limited due to low electric conductivity of sulfur and “shuttle effect” caused by diffusion of soluble polysulfides to the anode. In this study, self-made mesoporous TiO 2 and commercial Ketjen Black are mixed to obtain a composite material, which is then coated on glass fiber membrane through a slurry method. The modified glass fiber membrane is used as a functional separator in lithium-sulfur battery. The batteries using modified separator show a high initial discharge specific capacity of 1130.3mAh g −1 at 0.2C and an excellent cycling stability of 991.8mAh g −1 even after 60 cycles, and initial discharge specific capacity of 996.7mAh g −1 at 0.5C and 804.3mAh g −1 even after 100 cycles. The improved performance of the battery can be ascribed to effective adsorption of mesoporous TiO 2 to the soluble polysulfides and limit diffusion of the reaction intermediate to anode side . Moreover, the excellent electrical conductivity of Ketjen Black coated on the surface of glass fiber membrane can reduce the internal resistance, activate the absorbed polysulfides, and increase the specific capacity of the lithium-sulfur battery. It is believed that mesoporous TiO 2 and Ketjen Black modified glass fiber membrane effectively suppresses the “shuttle effect” during the cycling and provides a promising approach for high-performance lithium-sulfur batteries.

研究领域: 电化学 · 能源材料 · 纳米材料 · 电池技术 · 表面科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Mott-Schottky electrocatalyst selectively mediates the sulfur species conversion in lithium-sulfur batteries

Wenjie Ma,Zhitao Shao,Jing Yao,Kaixin Zhao,Xinzhi Ma,Lili Wu,Xitian Zhang

The lithium sulfur (Li-S) battery is an active research area in the field of energy storage systems, but the shuttle effect is a serious obstacle hindering its application. Herein, a CoSe 2 /CoO Mott-Schottky catalyst is blended with carbon nanotubes (CNTs) and subsequently coated onto a commercial separator as a modifier, whereby the synergy between the high electrocatalytic activity of the CoSe 2 /CoO heterostructure and high conductivity of the CNTs selectively mediate the conversion of sulfur species. As a result, a cell with a CoSe 2 /CoO-CNTs modified separator displays a high initial discharge capacity of 1573 and 910 mAh/g at 0.1 and 2C, respectively. Furthermore, a low decay rate of 0.070% per cycle can be obtained over 500 cycles at 2C. The results of this study suggest that the as-prepared CoSe 2 /CoO-CNTs is an effective modifier that can improve the performance of Li-S batteries for use in next-generation energy storage systems. This study provides fundamental insights into the rational design of Mott-Schottky catalysts for practical high-performance Li-S batteries.

研究领域: 电化学 · 能源材料 · 纳米材料 · 催化化学 · 储能技术
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WATER SCIENCE AND TECHNOLOGY · 2023 ·Vol. 87 ·期 11 ·2905-2916 · IF 2.7

Degradation of tetracycline by activated peroxodisulfate using a sulfur-modified iron-based material

Gao Shanxue,Zhang Nan,Chen Lei

View large Download slide View large Download slide Close modal The activation of persulfate by an iron-based catalyst presents a promising approach for the degradation of antibiotics; however, the activation efficiency remains a challenge. Herein, a sulfur-modified iron-based catalyst (S–Fe) by co-precipitation of sodium thiosulfate and ferrous sulfate in a molar ratio of 1:2 was prepared and the efficacy of the S–Fe/PDS system for the removal of tetracycline (TCH) was studied, where a higher removal efficiency was observed compared to the Fe/PDS system. Moreover, the effects of TCH concentration, PDS concentration, initial pH, and catalyst dosage on TCH removal were evaluated, and the highest efficiency was about 92.6% within a 30 min reaction time using a catalyst dosage of 1.0 g/L, a PDS dosage of 2.0 g/L, and a solution pH value of 7. The products and degradation pathways of TCH were analyzed by LC–MS. The free-radical-quenching experiments revealed that both SO 4 − • and •OH radicals contributed to the degradation of TCH in the S–Fe/PDS system, with the former playing a more significant role. The S–Fe catalyst also showed good stability and reusability for the removal of organic pollutants. Our findings suggest that the modification of an iron-based catalyst offers an effective approach to activate persulfate for removal of tetracycline antibiotics. The sulfur-modified iron-based catalyst (S–Fe) was prepared. Both SO 4 − • and •OH radicals played the role in the degradation of TCH in the S–Fe/PDS system. The S–Fe catalyst showed high catalytic activity and reusability for the removal of organic pollutants.

研究领域: 环境科学 · 催化化学 · 水污染治理 · 分析化学
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Gelatin-polyethylenimine composite as a functional binder for highly stable lithium-sulfur batteries

Naseem Akhtar,Hongyuan Shao,Fei Ai,Yuepeng Guan,Qifan Peng,Hao Zhang,Weikun Wang,Anbang Wang,Bingyin Jiang,Yaqin Huang

Lithium-sulfur (Li-S) batteries with high specific capacity are expected to be a new generation of energy storage devices. However, the shuttle effect of lithium polysulfide makes it difficult to commercialize stable Li-S batteries. In this work, we designed a gelatin-polyethylenimine composite (GPC) as functional binder for Li-S batteries to improve the stability of electrode during discharge-charge process. GPC binder combines the dispersion and adhesion ability of gelatin, which keeps cathode homogeneous and stable during electrochemical reaction , and adsorption capability of PEI for polysulfide , which suppresses the “shuttling effect”. The result shows that GPC used as a binder remarkably enhanced cyclic performance of Li-S battery with good capacity retention of about 100% at current density of 1C (sulfur loading 1.5 mg cm −2 ) after 100 cycles. We believe that GPC would be a promising binder for highly stable Li-S batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 纳米复合材料
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JOURNAL OF ORGANIC CHEMISTRY · 2024 · IF 3.3

Copper-Catalyzed Three-Component Synthesis of β-Hydroxysulfides from Styrene Oxide, Aryl Iodide, and Carbon Disulfide

Enbo Yu,Jun Li,Yue Wang,Ya Chen,Fuhong Xiao,Guo-Jun Deng

A copper-catalyzed three-component coupling reaction of styrene oxide, aryl iodide, and carbon disulfide for the construction of β-hydroxysulfides has been developed. In this process, readily available CS2 was used as the sulfur source to construct C–S bonds for the synthesis of phenyl-β-hydroxysulfides and (benzo[d]thiazol)-β-hydroxysulfides. This process features mild reaction conditions, simple operation, and wide substrate scope (>50 examples).

研究领域: 有机化学 · 合成化学
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Analytical Methods · 2019 ·Vol. 11 ·期 10 ·1353-1360 · IF 2.378

Sensitive and fast analysis of terbutaline sulfate in food using a modified electrode based on a MoS2/AuNPs nanocomposite

Xiaoyun Lin,Yanfang Wang,Miaomiao Zou,Yongnian Ni

Terbutaline sulfate (TBS) is a β2-adrenoceptor agonist, overdoses of which can cause serious harm and even be life-threatening to humans. Herein, we demonstrate a simple and facile method for the preparation of a molybdenum disulfide–gold nanoparticle composite (MoS2/AuNPs). The obtained MoS2 and MoS2/AuNPs were characterized and investigated by X-ray powder diffraction, scanning electron microscopy, and transmission electron microscopy. An MoS2/AuNPs-modified glassy carbon electrode (MoS2/AuNPs/GCE) was constructed using the dropping method and used to study the electrochemical behavior of TBS. The results indicated that the sensor had excellent electrocatalytic activity for TBS, with detection sensitivity for TBS more than 100 times higher compared with the bare GCE. With the successive addition of TBS, the peak current of the differential pulse stripping voltammogram (DPSV) of TBS was proportional to its concentration within a certain range, with a linear range of 1–85 nmol L−1 and limit of detection (LOD) of up to 0.47 nmol L−1. Furthermore, the modified electrode showed good stability, reproducibility, and anti-interference ability, meaning that it could be used to detect TBS in real samples.

研究领域: 分析化学 · 食品科学 · 电化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2013 · IF 2.206

Preparation of Two Dimensional Atomic Crystals BN, WS2, and MoS2 by Supercritical CO2 Assisted with Ultrasound

Yan Wang,Chenghong Zhou,Wucong Wang,Yaping Zhao

A facile and general approach was developed to exfoliate layer materials to produce two-dimensional atomic crystals. A single and few layers of BN, MoS2, and WS2 were obtained via directly exfoliating their powder materials using supercritical CO2 assisted with ultrasound. The effects of supercritical CO2 coupled with ultrasound play a key role in the exfoliation process. The layer numbers and sizes of the BN, MoS2, and WS2 can be easily controlled by adjusting the power and the time of ultrasonication. The AFM images suggest single-layered BN, MoS2, and WS2 were produced, respectively. Their lateral sizes are about 0.5–2 μm, and almost 90% of the BN sheets are less than five layers. The electric diffraction patterns demonstrate that the crystallinities of the produced samples remained the same as that of the raw material during the exfoliating process. This novel technique is cost-effective and scalable, and can be widely used in the production of two-dimensional atomic crystals with high quality.

研究领域: 材料科学 · 纳米科技 · 物理化学 · 表面科学 · 凝聚态物理
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Applied Sciences-Basel · 2017 ·Vol. 7 ·期 10 ·1036 · IF 1.679

Macroporous Activated Carbon Derived from Rapeseed Shell for Lithium–Sulfur Batteries

Mingbo Zheng,Qin Hu,Songtao Zhang,Hao Tang,Lulu Li,Huan Pang

Lithium–sulfur batteries have drawn considerable attention because of their extremely high energy density. Activated carbon (AC) is an ideal matrix for sulfur because of its high specific surface area, large pore volume, small-size nanopores, and simple preparation. In this work, through KOH activation, AC materials with different porous structure parameters were prepared using waste rapeseed shells as precursors. Effects of KOH amount, activated temperature, and activated time on pore structure parameters of ACs were studied. AC sample with optimal pore structure parameters was investigated as sulfur host materials. Applied in lithium–sulfur batteries, the AC/S composite (60 wt % sulfur) exhibited a high specific capacity of 1065 mAh g−1at 200 mA g−1and a good capacity retention of 49% after 1000 cycles at 1600 mA g−1. The key factor for good cycling stability involves the restraining effect of small-sized nanopores of the AC framework on the diffusion of polysulfides to bulk electrolyte and the loss of the active material sulfur. Results demonstrated that AC materials derived from rapeseed shells are promising materials for sulfur loading.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 可持续材料 · 电池技术
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Small · 2024 ·Vol. 20 ·期 40 ·2402725 · IF 13

A Universal Electronic Structure Modulation Strategy: Is Strong Adsorption Always Correlated with High Catalysis?

Mengyu Liu,Ruohan Hou,Pengpeng Zhang,Yukun Li,Guosheng Shao,Peng Zhang

Unveiling the inherent link between polysulfide adsorption and catalytic activity is key to achieving optimal performance in Lithium-sulfur (Li-S) batteries. Current research on the sulfur reaction process mainly relies on the strong adsorption of catalysts to confine lithium polysulfides (LiPSs) to the cathode side, effectively suppressing the shuttle effect of polysulfides. However, is strong adsorption always correlated with high catalysis? The inherent relationship between adsorption and catalytic activity remains unclear, limiting the in-depth exploration and rational design of catalysts. Herein, the correlation between “d-band center-adsorption strength-catalytic activity” in porous carbon nanofiber catalysts embedded with different transition metals (M-PCNF-3, M = Fe, Co, Ni, Cu) is systematically investigated, combining the d-band center theory and the Sabatier principle. Theoretical calculations and experimental analysis results indicate that Co-PCNF-3 electrocatalyst with appropriate d-band center positions exhibits moderate adsorption capability and the highest catalytic conversion activity for LiPSs, validating the Sabatier relationship in Li-S battery electrocatalysts. These findings provide indispensable guidelines for the rational design of more durable cathode catalysts for Li-S batteries.

研究领域: 电化学 · 材料科学 · 能源化学 · 纳米催化 · 电池技术
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