Surfaces and Interfaces
·
2025
·
IF 6.3
Fengxin Li,Yan Wang,Fumin Li,Mingqing Hua,Yan Huang,Huifang Cheng,Haibo Wu,Jiacheng Li,Jixing Liu
High-sulfur petroleum coke (HSPC), produced during petroleum coking process, has drawn ever increasing attention in the manufacture of graphite electrodes with the rise of new energy vehicles in recent years. However, its high sulfur content ( S > 3.0 wt.%) has become the major obstacle limiting this promising application. Herein, an innovative method is proposed to effectively lower the content of sulfur in HSPC through a series of polyoxometalate H 11 P 2 W 13 V 5 O 62 (HPA) coupled CeO 2 . The experimental results unveiled that the sulfur compounds in HSPC predominately existed as thiophene and mercaptan sulfur compounds, which could be oxidized to be the corresponding sulphone, sulphoxide and sulphate species. Moreover, the introduction of CeO 2 considerably promoted the dispersion of HPA, thereby exposing more reactive sites for the adsorption and activation of H 2 O 2 to produce active oxygen species, and thereafter endowing x%HPA@CeO 2 ( x = 20∼40) with excellent catalytic oxidative desulfurization (ODS) performance for HSPC. As a result, the sulfur content was significantly reduced from 4.46 wt.% to 2.12 wt.% at 70 °C and reaction time of 4 h due to the coupling effect between HPA and CeO 2 over 30%HPA@CeO 2 . The present study not only provides an innovative technological path for the efficient removal of sulfur from HSPC, but also promotes the understanding of catalytic ODS process of HSPC on the catalyst surface active centers.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Jiabei Gao,Weiquan Zhan,Ziwei Xiang,Shaoxian Song,José Luis Arauz-Lara,Feifei Jia,Peng Chen
Trace gold(I) recovery from thiosulfate solutions limits the application of thiosulfate leaching instead cyanide leaching method in industries. Here, facet engineering in cadmium sulfide (CdS) was proposed for trace gold(I) recovery from thiosulfate solutions (Au(S 2 O 3 ) 2 3− ). CdS nanomaterials with various exposing facets were obtained through adjusting the sulfur sources in hydrothermal synthesis process. It was found that Au(S 2 O 3 ) 2 3− recovery could reach 98.62 % under low concentration conditions, with a max reduction capacity of 204.95 mg/g. Besides, the recovery form of Au(S 2 O 3 ) 2 3− on CdS was metallic gold, realizing the reduction and recovery at the same time. The solution pH, sample dosage, S 2 O 3 2− , SO 3 2− , and ammonia ions as variants were considered to optimize the recovery performances. Even under the existence of interfered ions, the recovery kept very high. Au(S 2 O 3 ) 2 3− reduction on CdS was attributed to catalytic and chemical reduction. High exposed (0 0 2) facet content of CdS enhanced photocurrent intensity, thus improving Au(S 2 O 3 ) 2 3− reduction and recovery. Therefore, the work paved a way to realize trace gold(I) recovery from thiosulfate solutions via structure engineering in CdS, being expected to promote the application of thiosulfate leaching method.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Jianfei Wang,Wenwei Liu,Haiyang Jiang,Chen Li,Haoran Song,Shugen Liu,Yingjie Li,Senlin Tian,Ping Ning
Air pollution by sulfur dioxide (SO 2 ) remains a pressing concern for both the environment and human health. Desulfurization enhanced by persulfate based advanced oxidation processes (PS-AOPs) has been proven to be a feasible method. However, the inherent contradiction between the rapid diffusion mass transfer of SO 2 in the “gas-liquid-gas” phase and the limited lifespan of reactive oxygen species (ROS) can not be ignored. Excessive investment in PS is required to sustainably generate ROS to achieve continuous desulfurization performance, which may lead to excessive PS consumption. To address this issue, whether PS can achieve the oxidation absorption of SO 2 via a non-reactive oxygen species pathway was investigated. Experimental and computational results demonstrated that peroxymonosulfate (PMS) instead of peroxydisulfate (PDS) had a great SO 2 removal performance, the utilization of PS could be effectively achieved by maintaining a 1:1 molar ratio of PMS and removed SO 2 . The presence of H O O bonds in the PMS introduced a partial positive charge to the oxygen atom, making the PMS polar and more susceptible to be attacked by the nucleophile HSO 3 - . So SO 2 underwent a series of processes including dissolution, dissociation, one-oxygen atom transfer, and ionization before ultimately being converted into SO 4 2- ions, effectively achieving its removal from flue gas . This study may presents a novel approach for achieving high-efficiency flue gas desulfurization.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Jingui Han,Zhitao Shao,Yaozu Jia,Peiyao Liu,Zuqi Han,Xitian Zhang,Lili Wu,Xinzhi Ma
The practical applications of lithium–sulfur (Li–S) batteries have been significantly impeded by the heavy shuttle effect and slow bidirectional conversion of lithium polysulfides (LiPSs). In this study, a hierarchical NiS2/1T-MoS2 nanocomposite is utilized as a functionalized separator modifier to overcome the challenges. The MoS2 nanosheets are vertically and uniformly aligned on the surface of NiS2 microspheres, constructing a hierarchical yolk–shell structure. The NiS2 support not only significantly reduces the agglomeration of MoS2 nanosheets but also effectively stabilizes their 1T-phase structure, which is highly desirable for high-performance Li–S batteries. The Li–S battery with the NiS2/MoS2–CNT-modified separator delivers an excellent initial specific capacity of 1228 mA h g–1 at 0.2 C with a high-capacity retention of 85% over 100 cycles. It even achieves a discharge capacity of 722 mA h g–1 at 5 C. Furthermore, it maintains remarkable cycling stability with only 0.051% capacity decay per cycle during the long-term cycles at 1 C. This study not only provides a viable scheme for separator modifier design toward advanced Li–S batteries but also offers a universal route for stabilizing the 1T-phase structure of MoS2.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yu Ma,Yujia Ouyang,Huanyu Liang,Ping Li,Jing Shi,Jingyi Wu,Shuai Liu,Jingwei Chen,Yue Zhu,Huanlei Wang
Metallic sulfides are currently considered as ideal anode materials for potassium-ion batteries by virtue of their high specific capacities. However, their low intrinsic electronic conductivity, large volume variation and dissolution of polysulfides in electrochemical reactions hinder their further development toward practical applications. Here, we propose an effective structural design strategy by encapsulating CoS 2 /SnS 2 in sulfur-doped carbon layers, in which internal voids are created to relieve the strain in the CoS 2 /SnS 2 core, while the sulfur-doped carbon layer serves to improve the electron transport and inhibit the dissolution of polysulfides. These features enable the as-designed anode to deliver a high specific capacity (520 mAh/g at 0.1 A/g), a high rate capability (185 mA h g −1 at 10 A/g) and lifespan (0.016 % capacity loss per cycle up to 1500 cycles). Our comprehensive electrochemical characterization reveals that the heterostructure of CoS 2 /SnS 2 not only promotes charge transfer at its interfaces, but also enhances the rate of K + diffusion. Additionally, potassium-ion capacitors based on this novel anode are able to attain an energy density up to 162 Wh kg −1 and ∼ 96 % capacity retention after 3000 cycles at 10 A/g. The demonstrated design rule combining morphological and structural engineering strategies sheds light on the development of advanced electrodes for high performance potassium-based energy storage devices.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 40
·31629-31636
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IF 3.84
Yajin Hao,Zhiqiang Shi,Jing Wang,Qiang Xu
Nitrogen doped mesoporous carbon (NMC) with high specific surface area, large pore volume and stable nitrogen content has been prepared by in situ doping through one step carbonization to immobilize sulfur for lithium–sulfur batteries. The structure and composition of the prepared NMC and NMC@S composites are confirmed with nitrogen sorption, elemental analysis, X-ray photoelectron spectroscopy (XPS), X-ray diffraction patterns (XRD), high resolution transmission electron microscopy (HR-TEM) and thermogravimetric analysis (TGA). Scanning electron microscopy (SEM) images show a homogeneous distribution of sulfur within NMC@S. In comparison with free doped mesoporous carbon (MC), the NMC@S with high sulfur content (65%) is found to exhibit a higher initial discharge capacity of 1012 mA h g−1 and higher capacity retention. The electrochemical performance of Li–S batteries is improved by the nitrogen doping, which not only enhances the electric conductivity but also further confines polysufides to the mesoporous carbon from shuttle effect.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiafeng Ding,Yinan Zhang,Shihuan Lu,Xiaofang Zhang,Yan Li,Yuchi Zhong,Hangjun Zhang
Efficient and environmentally friendly methods for the remediation of polychlorinated biphenyls (PCBs)-contaminated wastewater have become an important issue. In this study, persulfate (PS) was activated with sodium thiosulfate (TS) to degrade 2,2′-dichlorobiphenyl (DCB) at an extraordinarily high rate at pH ≤ 4.0 at room temperature. The PS/TS system exhibited much higher activity than systems with PS or TS alone at pH 2.0: 90.3% DCB was removed within 120 min, a much higher removal rate than those of the latter systems. Sulfate radical (SO 4 − ) was verified to be the main reactive substance through scavenging and trapping experiments; sulfate radicals can decompose and detoxify DCB by dechlorination and hydroxylation processes. The removal efficiency of DCB (58.5% in 120 min) was also satisfactory in the TS system, in which TS could perform nucleophilic substitution on the DCB molecule at pH ≤ 4.0, followed by DCB dechlorination and the generation of hydroxy-biphenyl. Plausible mechanisms and reaction pathways involving nucleophilic substitution in the TS system and the formation of reactive oxygen species (ROS) in the PS/TS system to attack the carbon atom on DCB were proposed and calculated by density functional theory (DFT). The presence of Cl − , NO 3 − , HCO 3 − and humic acid (HA) may have inhibited the removal of DCB in the PS/TS system, while the effect was not significant in the TS system. Our work introduces novel and rapid removal methods for the removal of PCBs and may be significant for the development of efficient strategies for halogenated pollutant control in real water.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 20
·6876-6883
·
IF 4.174
Zhe Cui,Shu-Ang He,Qian Liu,Rujia Zou
Herein, a simple approach was developed to fabricate novel NiCo2O4 hollow nanoflowers (NCOHFs), which were explored as a sulfur carrier material for lithium–sulfur (Li–S) batteries. Remarkably, the capacity of the NCOHF/S composite electrode was ∼666.8 mA h g−1 in the fourth cycle, which was maintained at ∼432.9 mA h g−1 in the 400th cycle under a current density of 1.0C, with a low decay rate of 0.087% per cycle. The overall outstanding properties of the NCOHF/S composite are attributed to the successful new strategy in structural design via in situ and ex situ procedures. Firstly, NCOHF with bifunctional catalytic activity and chemical adsorption can efficiently promote the redox reactions of lithium polysulfides (LiPSs) and suppress the diffusion of polysulfides. Secondly, NCOHF with inherently high electronic conductivity acts as a conduit to accelerate the transport of electrons and ions. Thirdly, the flower-like NiCo2O4 nanosheets are anchored tightly to the conductive carbon and binder during the Li+ insertion and extraction processes, which can effectively suppress the aggregation of the NCOHF/S composite during cycling. Finally, the hollow space inside the NCOHF/S composite provides sufficient free space for the expansion of encapsulated pure sulfur.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Tong Wu,Guiru Sun,Wei Lu,Liping Zhao,Alain Mauger,Christian M. Julien,Liqun Sun,Haiming Xie,Jinghai Liu
The inhibition of the shuttle of lithium polysulfides (LiPSs) and enhancement of the electrical conductivity of the cathodes are desirable to improve the performance of lithium-sulfur batteries. In the present work, we report a cathode acting simultaneously as a highly efficient LiPSs immobilizer and sulfur host. It is composed of sulfur embedded inside a hollow sphere, the shell of which is made of hollow black TiO 2 (b-TiO 2 ) spherical nanoparticles . The particles of the composite are then coated with a polypyrrole (PPy) layer to form the active cathode element (b-TiO 2 /S@PPy). The particular topology of the b-TiO 2 layer provides enough space to alleviate the volume expansion of LiPSs. Equally, the PPy coating layer can not only improve the conductivity of the cathodes, but also restrain the shuttle of LiPSs by chemical adsorption . With the sulfur content of 59.6 wt% corresponding to a sulfur loading of 1.5–1.8 mg cm −2 , the lithium-sulfur batteries with the b-TiO 2 /S@PPy cathode exhibits a high initial discharge capacity (1374 mAh g −1 at 0.1C), a superior cycling stability (910 mAh g −1 after 200 cycles at 0.1C), and a good rate performance (725 mAh g −1 at 2C).
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
He Yang,Xu Zhang,Junling Guo,Weili Zhu,Shupeng Zhao,Fang Wang,Qiuyu Fan,Hongyan Xiao,Fengxiang Zhang
Lithium sulfur (Li-S) battery is considered as one of promising energy-storage devices owing to its high energy density and low cost. However, it is still a great challenge to explore stable sulfur cathode with high sulfur loading and good cycling performance. Herein, we report a facile method to prepare N,S co-doped hierarchical pore structured carbon foam @porous carbon (CF@N-SPC) through a carbonation process from resin aerogel coated melamine foam with thiourea as the source for N and S codoping. The close combination of a carbon interconnected skeleton and the resin aerogel derived carbon forms the hierarchical pore structure that improves the electron and ion transport. The prepared CF@N-SPC can be used as a freestanding cathode without a conductive additive and a binder. Due to the synergistic effect of the hierarchical pore structure and N, S codoping, the sulfur loading in the carbon foam-based cathode can reach up to 10.6 mg cm −2 . Owing to these unique merits, the CF@N-SPC/S cathode exhibits high capacity and good cycling performance: it yields a discharge capacity of 1212 mA h g −1 at 0.1 C with 4.0 mg cm −2 sulfur loading; it also exhibits a good discharge capacity of 668 mA h g −1 at 0.5 C when the sulfur loading increases to 10.6 mg cm −2 , capacity retained by 72% in 200 cycles; it experiences a very small capacity decay rate of 0.05% per cycle in 700 cycles at 1 C. Our rational design and facile synthesis of the carbon foam-based freestanding cathode is promising and applicable for development of high performance Li-S batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
2019
·Vol. 6
·期 9
·2570-2577
·
IF 3.975
Yang Hua,Xueliang Li,Xingchi Zhang,Luyao Zhang,Yizhen Shu,Huijuan Sheng,Huagao Fang,Haibing Wei,Yunsheng Ding
Graphical Anchored down : Ultrafine ZnS is successfully introduced into carbon aerogel (CA) to form a cathode for lithium–sulfur batteries. The nanoporous ZnS-CA composites present excellent electrochemical performances, owing to the ZnS nanoparticles having a strong affinity for Li 2 S n species. Furthermore, the strong affinity was validated by first-principles theory calculations; the results clearly reveal the anchoring and catalytic mechanism. A carbon aerogel composite modified with ZnS (ZnS-CA) was successfully prepared through a simple in situ synthesis and used as a cathode for lithium-sulfur batteries. The nanopore ZnS-CA composites with a high specific surface area and rich mesoporous structure exhibit stronger adsorption and immobilization ability for polysulfides. The ZnS-CA/S cathode materials offer excellent electrochemical performances with lasting cycling stability and high specific capacity. In particular, the 6ZnS-CA/S sample achieves an initial capacity of 1352 mAh g −1 at 0.2 C and maintains a high capacity of 1119 mAh g −1 after 100 cycles. Furthermore, after 300 long cycles, it still maintains a high capacity of 730 mAh g −1 at 1 C. These excellent performance features are attributed to the strong affinity of ZnS for Li 2 S n species, thus polysulfide shuttling can be effectively inhibited from the cathode source. Furthermore, the strong adsorption energy between ZnS and polysulfides was validated by using first-principles theory calculations, which reveals the anchoring and catalytic mechanism.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2014
·
IF 5.211
Xiaoyan Liu,Zhongqiang Shan,Kunlei Zhu,Jiangyong Du,Qiwei Tang,Jianhua Tian
Lithium sulfur batteries have brought significant advancement to the current state-of-art battery technologies due to their high theoretical specific energy of 1675 mAh g −1 . However, the rapid capacity degradation, mainly caused by polysulfide dissolution, remains a significant challenge prior to practical applications. In this work, a sulfur cathode modified by bifunctional nafion/γ-Al 2 O 3 membrane has been successfully prepared, which can remarkably immobilize the polysulfides within the unique cathode structure due to its ions selectivity and absorbent capacity. A high initial discharge capacity of 1448.0 mAh g −1 can be achieved at 1C and 788.6 mAh g −1 preserved after 200 cycles, indicating a slow degradation. Furthermore, the coulombic efficiency maintains as high as 97% during cycling. The excellent electrochemical properties can be attributed to the bifunctional and stable membrane which can dramatically reduce the shuttle effect and keep integrated even after charging–discharging for 200 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）