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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2020 ·Vol. 167 ·期 12 ·122511 · IF 3.721

Communication—Electrolysis of Metal Sulfides in Sulfur-Containing Carbon Saturated Iron Melt

Zhihao Lu,Chengjun Liu,Yingying Yue

In this paper, the feasibility of electrolysis of Cu2S and FeS in sulfur-containing carbon saturated iron melt aided by liquid lead cathode is studied by cyclic voltammetry and potentiostatic electrolysis at 1300 °C. The Cu2S and FeS are electro-reduced on the lead cathode and the product copper dissolve into the liquid lead while the product iron dissolves into iron melt due to the difference of solubility. An insert graphite rod in iron melt was used as the anode, on which the S2− is oxidized to S. This finding provides a new way for refining sulfide impurities in iron-based melt.

研究领域: 冶金学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Cooperative catalytic Mo-S-Co heterojunctions with sulfur vacancies for kinetically boosted lithium-sulfur battery

Haobin Song,Tong Li,Tingting He,Zhouhao Wang,Daliang Fang,Ye Wang,Xue Liang Li,Daohong Zhang,Junping Hu,Shaozhuan Huang

The intelligent design of catalytic materials with unique architectures has a significant impact on regulating the polysulfides (LiPSs) conversion and boosting the performance of Li − S batteries. Here, starting from 2D catalytic MoS 2 nanosheets and combined with the first-principle calculations, the covalent heterojunction and S vacancy are simultaneously developed in MoS 2 to regulate the electronic structure and improve the LiPSs conversion kinetics. The S vacancy and heterojunction (MoS 2-x -Co 9 S 8-y ) engineering can significantly improve the electrical conductivity of MoS 2 by incorporating shallow donor levels into the MoS 2 . Moreover, the incorporation of Co 9 S 8-y greatly improves the chemisorption ability of heterostructure towards LiPSs. The LiPSs are preferentially adsorbed at the catalytic Mo-S-Co heterojunction, where both Li + and e - are easy to access. The coupled fast Li + /e - transportation of MoS 2-x -Co 9 S 8-y enables direct and fast LiPSs “adsorption-conversion” at the catalytic Mo-S-Co heterojunction with enhanced bidirectional catalytic properties. Due to the ingenious co-engineering of S vacancy and heterointerface, the Li − S cell with MoS 2-x -Co 9 S 8-y /rGO interlayer delivers high sulfur utilization (1382.5 mAh/g at 0.1C), excellent rate capability (710.2 mAh/g at 3C), and long cycle life over 600 cycles (0.06 % capacity decay per cycle). This work demonstrates the great potential of anion deficiency and heterojunction co-construction for high-performance Li − S batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Improved extraction of acid-insoluble monosulfide minerals by stannous chloride reduction and its application to the separation of mono- and disulfide minerals in the presence of ferric iron

Han Ye,Kun Gao,Guining Lu,Yingying Xie,John R. Reinfelder,Weilin Huang,Xueqin Tao,Xiaoyun Yi,Zhi Dang

Metal sulfides, which are important indicators of sulfur cycling, are usually divided into two categories according to sulfur chemical valence: (1) monosulfides (S 2− ) and (2) disulfides (S 2 2− ). The two sulfur species are separated and quantified by a sequential-extraction method. Specifically, monosulfides are extracted as acid-volatile sulfide (AVS) using 6 M HCl prior to the extraction of disulfides using acidic CrCl 2 , which is defined as chromium-reducible sulfur (CRS). However, the conventional AVS procedure does not result in the quantitative extraction of S 2− from the acid-insoluble metal monosulfide, copper sulfide (CuS). Consequently, residual sulfur in CuS (CuS-S) may be extracted as CRS resulting in the inaccurate separation of these two sulfur species. In this study, we used stannous chloride (SnCl 2 ) to improve CuS-S recovery in the AVS procedure and permit the separate extraction of sulfur from CuS and pyrite (FeS 2 ), the most abundant disulfide in nature. Our results show that the addition of SnCl 2 increased the recovery of CuS-S as AVS from less than 36% to as high as 92% in the absence of pyrite and Fe 3+ and 89% in the presence of pyrite and Fe 3+ . In addition, based on the observed correlation between the concentration of SnCl 2 and the dissolution of FeS 2 , we identified the appropriate concentration of SnCl 2 needed to avoid the dissolution of FeS 2 in the AVS procedure. SnCl 2 also minimized the oxidation of CuS-S by Fe 3+ released from ferric minerals during the extraction of AVS. Based on the results of a series of sequential-extraction experiments, we show that an amendment of SnCl 2 in the AVS procedure followed by CRS permits the quantitative separation of CuS-S and FeS 2 -S while also preventing interference by Fe 3+ . Our method will find application in research concerned with the fate of metals and the biogeochemistry of sulfur in the environment.

CAS / MDL: 1317-40-4 7772-99-8
研究领域: 环境科学 · 矿物学 · 化学
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APPLIED SURFACE SCIENCE · 2018 · IF 4.439

The role of S(II) and Pb(II) in xanthate flotation of smithsonite: Surface properties and mechanism

Kai Jia,Qiming Feng,Guofan Zhang,Wanying Ji,Wukai Zhang,Bingqian Yang

Smithsonite is a readily dissolvable carbonate mineral that is naturally hydrophilic, making recovery of this ore by flotation difficult. The flotation results showed that conditioning with only sodium sulfide (Na 2 S) did not successfully allow the smithsonite samples to float, whereas treatment with a combination of S(II), Pb(II) and xanthate (with Na 2 S as the sulfurizing reagent, lead ions (Pb(II)) as the activator, and xanthate as the collector) improved the flotation of smithsonite, achieving a mass recovery of 95.8%. A combination of analytical techniques, including X-ray diffraction (XRD), atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS), in conjunction with depth profiling , was used to investigate the chemical nature of the sulfur and lead species on the smithsonite surface. For S(II)-conditioned smithsonite, a layer of ZnS formed on the smithsonite (ZnCO 3 ) substrates; this newly formed ZnS coating was amorphous or poorly crystallized. For smithsonite samples conditioned with S(II) and Pb(II), the microstructures and the phase constituents, obtained by AFM and XRD analyses, confirmed the formation of the PbS species with a cubic galena structure on the surface. XPS depth profiling showed that the PbS layer was 18-nm thick, which corresponds to 30 PbS molecular layers . This study presents direct evidence that the coating of the activation product, PbS, on the smithsonite surface was similar to a relatively thick galena layer, which led to successful flotation.

CAS / MDL: 1310-73-2 7647-01-0
研究领域: 矿物学 · 材料科学 · 化学工程
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Microscale exploration of the sulfidization flotation theory in malachite

Qiming Zhuo,Panpan Wang,Peilun Shen,Penghui Wang,Yongqi Tian,Decheng Chen,Jiushuai Deng,Wenli Liu

With the gradual depletion of copper sulfide resources, efficient flotation technologies for the recovery of copper oxide minerals, such as malachite, have received significant attention. Although sulfidization plays a critical role in malachite flotation, the fundamental theory of sulfidization flotation remains uncertain in the context of practical industrial applications. In this study, evolution of the sulfide product morphology on the malachite surface was observed after treatment with various concentrations of sodium sulfide. In addition, the valence states and phase compositions of the sulfide products were investigated using different X-ray techniques. Furthermore, the evolution of the malachite surface morphology after the formation of a sulfide film was investigated, as were the interaction forces between the malachite and bubbles under the action of butyl xanthate. As a result, it was possible to directly observe the growth process of the sulfide film on the malachite surface, and the presence of Cu(I) was confirmed in the sulfide products. Moreover, the compositions of the sulfide products were investigated using X-ray techniques. The obtained results demonstrated that the sulfide film facilitated the formation of butyl xanthate product layers on the malachite surface, whilst also enhancing the interfacial interaction forces between the malachite and the bubbles.

CAS / MDL: 871-58-9 1313-84-4
研究领域: 矿物加工工程 · 材料科学与工程
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Journal of Energy Chemistry · 2022 · IF 13.599

Single-phase bimetal sulfide or metal sulfide heterojunction: Which one is better for reversible oxygen electrocatalyst?

Jingjing Cai,Huijun Liu,Yulin Luo,Yuqing Xiong,Lizhu Zhang,Sheng Wang,Kang Xiao,Zhao-Qing Liu

Bimetallic sulfides, integrating the merits of individual components, are ideal structures for efficient electrocatalysis. However, for bimetallic sulfides including metal sulfide heterojunctions (MSH) and single-phase bimetallic sulfides (SBS), it is still unclear about which one has better catalytic activity toward reversible oxygen catalysis and its difference on catalytic mechanism. In this work, we demonstrate a bimetallic sulfide electrocatalyst that could transform from metal sulfide heterojunction (CoS/FeS) to single-phase bimetallic sulfide (CoFeS 2 ) through a facile temperature control strategy. The single-phase bimetallic sulfide (CoFeS 2 ) affords high intrinsic activity, fast reaction kinetics and superior durability toward oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Density functional theory (DFT) simulations reveal that the (CoFeS 2 ) has homogeneous electron distribution of the CoFeS 2 structure, improves the central energy level of d band, and optimizes the O* and OOH* intermediate and efficiently reduces the energy barrier of the reaction rate-determining step (RDS). The assembled rechargeable zinc-air battery is more stable than the Pt/C and IrO 2 assemblies due to the excellent electrocatalytic activity and stability of CoFeS 2 /NC, suggesting that it has potential for use in practical applications.

研究领域: 材料科学 · 电化学 · 理论计算
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 7 ·3834-3844 · IF 11.301

Ni3S2 anchored to N/S co-doped reduced graphene oxide with highly pleated structure as a sulfur host for lithium–sulfur batteries

Daying Guo,Zihe Zhang,Bin Xi,Zhisheng Yu,Zhen Zhou,Xi'an Chen

Reported herein is the investigation of a unique cathode candidate for Li–S batteries, i.e. Ni3S2/(N, S)-RGO-type hybrid materials, which are expected to optimize battery performance by elevating the utilization of sulfur and chemically confining the adsorption/diffusion of polysulfide. Versatile structural and compositional characterizations confirmed the uniform growth and strong chemical coupling of nanostructured Ni3S2 on the N/S co-doped RGO matrix. Rich physical and chemical properties were revealed, namely, the large specific surface area and pore volume, which are beneficial for polysulfide capture, and the 3D conductive network supporting rapid charge transfer to the Ni3S2-polysulfide interface to improve the intrinsic equilibrium of the polysulfide. Specifically, the integration of ∼28.2 wt% of Ni3S2 produced a highly pleated composite with the largest BET specific surface area (618 m2 g−1) and pore volume (1.73 cm3 g−1) among the hybrids studied. This typical material also performed the best in the battery test, recording ultra-high cycling stability over 1000 cycles at the current density of 3C with the capacity decay of 0.023% per cycle. As the sulfur loading per unit area became as dense as 5.8 mg cm−2, the specific capacities were measured as 6.72 mA h cm−2 (at 0.05C), while the capacity retention for the 200-cycle test (at 1C) was still preserved above 72.5%.

研究领域: 材料科学 · 电化学 · 能源存储
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2019 · IF 4.084

One-pot synthesis of MoS2/CdS nanosphere heterostructures for efficient H2 evolution under visible light irradiation

Lei-Lei Li,Xing-Liang Yin,Dong-Hui Pang,Xin-Xin Du,Han Xue,Hua-Wei Zhou,Qing-Xia Yao,Huai-Wei Wang,Jun-Chao Qian,Jie Yang,Da-Cheng Li,Jian-Min Dou

Exploration of cost-efficient and high-performance photocatalyst for H 2 evolution by using a facile approach is of great importance. In this manuscript, a facile one-pot method was employed to fabricate MoS 2 /CdS heterostructures with MoS 2 intimately grown on the surface of CdS resulting in the formation of well-defined heterostructures. Screen experiment reveals the optimized photocatalytic H 2 evolution performance of MoS 2 /CdS is far exceeding that of pristine CdS by a factor of more than 162. The outstanding performance can be ascribed to the formation of heterostructures which accelerate charge transportation and separation, and the MoS 2 serving as a cocatalyst for the decrease of H 2 overpotential. Moreover, the photocatalytic mechanism of the MoS 2 /CdS was carefully investigated, which contributes to the deep understanding of the photocatalytic process and the designation of other low-cost and high-efficient photocatalyst.

研究领域: 材料科学 · 能源化学
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Nanomaterials · 2020 ·Vol. 10 ·期 4 ·774 · IF 4.324

Studies on Sensing Properties and Mechanism of CuO Nanoparticles to H2S Gas

Fang Peng,Yan Sun,Yue Lu,Weiwei Yu,Meiying Ge,Jichao Shi,Rui Cong,Jiaming Hao,Ning Dai

In this work, the high crystalline copper oxide (CuO) nanoparticles were fabricated by a hydrothermal method, and their structural properties were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The sensing results show that CuO nanoparticles exhibit enhanced sensitivity and good selectivity for hydrogen sulfide (H2S) gas at a low temperature. There are two working mechanisms involved in the H2S sensing based on CuO nanoparticle sensors. They are the H2S oxidation mechanism and the copper sulphide (CuS) formation mechanism, respectively. The two sensing mechanisms collectively enhance the sensor’s response in the H2S sensing process. The Cu–S bonding is stable and cannot break spontaneously at a low temperature. Therefore, the CuS formation inhibits the sensor’s recovery process. Such inhibition gradually enhances as the gas concentration increases from 0.2 ppm to 5 ppm, and it becomes weaker as the operating temperature rises from 40 °C to 250 °C. The XPS results confirmed the CuS formation phenomenon, and the micro Raman spectra demonstrated that the formation of CuS bonding and its decomposition can be effectively triggered by a thermal effect. Gas-sensing mechanism analysis supplied abundant cognition for the H2S sensing phenomena based on CuO materials.Keywords:CuO;H2S;mechanism;oxidation;CuS formation

CAS / MDL: 64-17-5 6046-93-1
研究领域: 材料科学 · 化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

Sulfide-induced reduction of nitrobenzene mediated by different size fractions of rice straw-derived black carbon: A key role played by reactive polysulfide species

Chenhui Wei,Shujun Yin,Heyun Fu,Xiaolei Qu,William A. Mitch,Dongqiang Zhu

Here we investigated the mediation efficiency of different size fractions of rice straw-derived black carbon (BC) using sulfide-induced nitrobenzene reduction as a model system. The bulk BC was divided into three size fractions: dissolved BC (size <0.45 μm), colloidal BC (0.45 μm < size < 1 μm), and particulate BC (size > 1 μm). With the presence of BC fractions (250 mg/L) nitrobenzene reduction by Na 2 S was significantly facilitated, wherein the mediation efficiency was positively correlated with the BC fraction's oxygen group content in an order of particulate BC < colloidal BC ≪ dissolved BC. Consistently, the oxidation treatment of particulate BC with O 3 or HNO 3 improved the mediation efficiency, whereas the reduction treatment with NaBH 4 reduced the mediation efficiency. The supernatant collected with dialysis or filtration of suspension of BC materials pre-reacted with Na 2 S could effectively reduce nitrobenzene, suggesting that reactive reducing sulfur species were produced in aqueous solutions by reacting sulfide only with BC materials. This was evidenced by the fact that polysulfides and polysulfide radicals were both detected in the supernatant. As demonstrated by electron paramagnetic resonance analysis, the quinone moieties at the surface of BC materials accepted electrons from sulfide and turned into semiquinone free radicals, consequently leading to formation of reactive reducing sulfur species and thus enhanced nitrobenzene reduction. The strong mediation efficiency on redox reactions observed for colloidal BC and dissolved BC combined with their significant mobility in subsurface environments indicate that these carbonaceous materials may play an important role in the fate process of organic contaminants as both carriers and catalysts. Capsule The surface quinone moieties of BC induce the formation of reactive reducing sulfur species by acting as one-electron acceptors and facilitate nitrobenzene reduction by sulfide.

CAS / MDL: 7704-34-9
研究领域: 环境科学 · 化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Dual-function LiFePO4 modified separator for low-overpotential and stable Li-S battery

Ming Jin,Rui Gao,Guiru Sun,Haibo Li,Xiangxin Xue,Chaoqun Qu,Nan Li,Yuting Zhang,Zhao Wang,Ming Feng

Lithium sulfide (Li 2 S) compounds as cathode materials for Lithium-sulfur (Li-S) battery have attracted more and more attention recently because of its high specific capacity, lower volume expansion and higher thermal stability of Li 2 S. However, high electrochemical barrier of the Li 2 S cathode and “shuttle effect” from S species on anode still block the development of Li-S batteries. Herein, LiFePO 4 (LFP) is employed as dual-function separator modifier to establish hybrid cathode. The modified separator will reduce overpotential for effective and durable sulfur redox reactions at the same time, it can also efficiently immobilize the lithium polysulfides (LiPSs) through the Lewis acid-base interaction of LiPSs and LFP. The battery systems based on the as-developed LFP modified separator exhibit an excellent rate capability, high sulfur utilization and outstanding cycling performance. The capacity retention can reach 83.9% after 400 cycles at 0.2 C, and the capacity can reach 594 mAh g −1 at up to 2 C. Current facile and low-cost strategy to modified Li-S battery systems on one hand offers an effective pathway to enhance electrochemical performance, on the other hand inspire new strategies on reducing the activation barrier of Li 2 S for improved sulfur electrochemistry as well.

CAS / MDL: 10377-48-7 872-50-4
研究领域: 材料科学 · 电化学 · 能源存储
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2018 · IF 4.229

Highly efficient hydrogen evolution catalysis based on MoS2/CdS/TiO2 porous composites

Jimin Du,Huiming Wang,Mengke Yang,Fangfang Zhang,Haoran Wu,Xuechun Cheng,Sijie Yuan,Bing Zhang,Kaidi Li,Yina Wang,Hyoyoung Lee

Efficient production of hydrogen through visible-light-driven water splitting mechanism using semiconductor-based composites has been identified as a promising strategy for converting light into clean H 2 fuel. However, researchers are facing lots of challenges such as light absorption and electron-hole pair recombination and so on. Here, new sheet-shaped MoS 2 and pyramid-shaped CdS in-situ co-grown on porous TiO 2 photocatalysts (MoS 2 CdS TiO 2 ) are successfully obtained via mild sulfuration of MoO 3 and CdO coexisted inside porous TiO 2 monolith by a hydrothermal route. The scanning electron microscopy and transmission electron microscopy results exhibit that the MoS 2 CdS TiO 2 composites have average pore size about 500 nm. The 3%MoS 2 10%CdS TiO 2 demonstrated excellent photocatalytic activity and high stability for a hydrogen production with a high H 2 -generation rate of 4146 μmol h −1  g −1 under visible light irradiation even without noble-metal co-catalysts. The super photocatalytic performance of the visible-light-driven hydrogen evolution is predominantly attributed to the synergistic effect . The conduction band of MoS 2 facilitates in transporting excited electrons from visible-light on CdS to the porous TiO 2 for catalytic hydrogen production, and holes to MoS 2 for inhibiting the photocorrosion of CdS, respectively, leading to enhancing the efficient separation of electrons and holes.

研究领域: 材料科学 · 能源科学
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