FUEL
·
2021
·
IF 6.609
Chengyang Cao,Yang Ren,Hao Wang,Hongyun Hu,Baojun Yi,Xian Li,Linling Wang,Hong Yao
Solar-powered pyrolysis of waste tires has been extensively studied because it can rapidly convert waste tires into valuable gas products using sustainable energy. However, the emitted sulfurous pollutants during this fast pyrolysis process would significantly reduce the economic feasibility of disposal waste tires. In order to investigate and regulate the sulfur transformation behavior, a large-load thermogravimetric analyzer and an optical rapid thermal processor were adopted to characterize and simulate the solar-powered fast pyrolysis behavior. The sulfur fixation effect of CaO was also evaluated in this study. Results showed that CaO addition could increase the emission of H 2 and CO by promoting the cracking of organic compounds in tar. In comparison, it could decrease the CO 2 emission by adsorption or transformation. Also, an excellent sulfur fixation rate in char was achieved with 10 wt% CaO addition, but accompanied by increasing emission tendency of SO 2 , especially at 650 °C-6000 °C/min. It was attributed to the competition reaction between H 2 S and SO 2 in the gas phase and interaction between CaS and CaSO 4 in the condensed phase. Our findings could be beneficial to develop an in-situ sulfur removal method during the pyrolysis of waste tires in the industry.
研究领域:
能源与环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
WASTE MANAGEMENT
·
2023
·
IF 8.1
Mengxin Lu,Yongjie Xue,Hui Zhao,Xiaoshan Zhang,Teng Wang
Secondary sulfur pollution in dyeing sludge (DS) during drying and incineration is a major environmental problem necessitating in-situ control. To robustly immobilise sulfur during drying–incineration, the authors introduce an electromagnetic induction (EMI) drying method and reveal the corresponding migration and conversion of sulfur in DS. The EMI-drying efficiency reached 10.69%/min, five times that of thermal drying. EMI drying increases the relative sulfoxide ratio from that of thermal drying. In a sludge–sulfur model, the proposed treatment promoted the oxidation and decomposition of organic sulfur without noticeably affecting the inorganic sulfur. The selective oxidation process during EMI drying promotes sulfur stabilisation in dried DS, decreasing the performance and stability of DS combustion. The sulfur-containing pollutants released during the incineration of DS mainly contain H 2 S, followed by CH 3 SH and SO 2 . EMI drying increases the outputs of SO 2 and CH 3 SH but decreases the outputs H 2 S and total sulfur compared with the outputs of thermal drying. Under the sulfur-model conditions, EMI promoted the conversion of inorganic sulfur to sulfur-containing gases (especially H 2 S) during incineration. In contrast, the sulfur stabilised by partial oxidation of organic sulfur in the EMI-dried DS was not easily converted to gaseous sulfur during subsequent combustion. Overall, EMI inhibits the release of sulfur during the combined drying–incineration process of DS.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Qizi Fu,Chenxi Li,Zirui Liu,Xingyu Ma,Yunhao Xu,Yan Wang,Xuran Liu,Dongbo Wang
Bisphenol A (BPA), as a typical leachable additive from microplastics and one of the most productive bulk chemicals, is widely distributed in sediments, sewers, and wastewater treatment plants, where active sulfur cycling takes place. However, the effect of BPA on sulfur transformation, particularly toxic H2S production, has been previously overlooked. This work found that BPA at environmentally relevant levels (i.e., 50–200 mg/kg total suspended solids, TSS) promoted the release of soluble sulfur compounds and increased H2S gas production by 14.3–31.9%. The tryptophan-like proteins of microbe extracellular polymeric substances (EPSs) can spontaneously adsorb BPA, which is an enthalpy-driven reaction (ΔH = −513.5 kJ mol–1, ΔS = −1.60 kJ mol–1K –1, and ΔG = −19.52 kJ mol–1 at 35 °C). This binding changed the composition and structure of EPSs, which improved the direct electron transfer capacity of EPSs, thereby promoting the bioprocesses of organic sulfur hydrolysis and sulfate reduction. In addition, BPA presence enriched the functional microbes (e.g., Desulfovibrio and Desulfuromonas) responsible for organic sulfur mineralization and inorganic sulfate reduction and increased the abundance of related genes involved in ATP-binding cassette transporters and sulfur metabolism (e.g., Sat and AspB), which promoted anaerobic sulfur transformation. This work deepens our understanding of the interaction between BPA and sulfur transformation occurring in anaerobic environments.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xiaoqing Lin,Canming Ma,Deli Wu
Metal-enhanced ozonation can greatly improve the decay of organic matter; however, whether this method benefits the decay of malodorous compounds or not and the possible mechanism are not well understood. In this study, nine typical malodorous compounds were selected to reveal that Cu(II)-enhanced ozonation can greatly promote the decay of fatty amines because of the direct ozone oxidation , which was enhanced to promote ozone utilization. Moreover, trace Cu(II) can amplify the observed rate constants of dimethylamine and trimethylamine for 48.9% and 155.7%, respectively, and Cu(II) dosage was the determining factor using response surface methodology to investigate the interactions between initial pH, Cu(II) dosage and ozone dosage. These results demonstrated that the formation of • OH and O 2 •– was inhibited rather than promoted, which was quite different from some previously reported Cu(II)-enhanced ozonation counterparts. Moreover, the enhanced effect of trace Cu(II) was exhibited in both single and complex malodorous compounds. The conversion pathway of nitrogen and sulfur elements was clarified, with the targeted mineralization of nitrogen of nitrogen-containing malodorous compounds into NO 3 -N and the odor characteristics of sulfur-containing malodorous compounds disappeared. These findings provided new insight for utilizing metal ions to enhance the direct ozone oxidation capacity of malodorous compounds.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2022
·
IF 4.132
Yucui Hou,Qi Zhang,Minjie Gao,Shuhang Ren,Weize Wu
The absorption of SO2 from flue gas and its conversion to chemicals is important in the industry. Functional ionic liquids (ILs) have been broadly used to absorb SO2 in flue gas, but seldom convert it to chemicals. As we know, water is inevitable in a desulfurization process. In this work, three functional ILs (monoethanolaminium lactate-[MEA][Lac], 1,1,3,3-tetramethylguanidinium lactate-[TMG][Lac], tetraethylammonium lactate-[N2222][Lac]) with or without water were used as absorbents to absorb SO2 in flue gas, and then the absorbed SO2 in the absorbents was converted to sulfur via a Claus reaction. The result shows that the three ILs can efficiently absorb SO2 and convert it to sulfur. But the addition of water in the ILs can reduce the conversion of absorbed SO2, and the conversion increases with increasing the acidity of absorbents. To explain this phenomenon, we studied the Claus reaction in H2SO3, NaHSO3 and Na2SO3 aqueous solutions. It turns out that the conversion of the Claus reaction is related to the species of S (IV) in the order of the oxidability: H2SO3 > HSO3– > SO32–, and their proportions dependent on the pH of solutions. On the basis of the absorption mechanism of SO2 in functional ILs aqueous solution, H2S reacts with HSO3– and SO32– with weaker oxidability, resulting in the lower conversion. Importantly, we found that the addition of lactic acid could increase the conversion of SO2 via the Claus reaction.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ying Wu,Yiyuan Xing,Xiaodan Zhao,Zuoming Zhou,Guohua Jing
Recently, activation of sulfite for production of sulfate radical (SO 4 •− ) has emerged for abatement of organic contaminants. Herein, with regard to the excellent activation efficacy of Co(II) and the enhanced electron donating capacity by sulfur species, cobalt sulfide (CoS) was proposed for efficient sulfite activation towards iohexol abatement via SO 4 •− –based advanced oxidation processes. CoS exhibited better activation performance than typical CoO and Co 3 O 4 with a sharp decline of iohexol within 0.5 min, for which superior electron transfer efficiency of CoS was confirmed by Electrochemical impedance spectroscopy (EIS). The contribution of SO 4 •− and HO • to iohexol abatement was demonstrated by radical quenching experiment and Electron paramagnetic resonance (EPR). The influences of various parameters (solution pH, CoS and sulfite dosage, iohexol concentration), co-existing anions (HCO 3 − , HPO 4 2− , Cl − and NO 3 − ) and humic acid on iohexol abatement were investigated, as well as, the effect of different water matrixes on iohexol abatement was also evaluated. A possible mechanism was proposed based on ionic strength experiment, Transmission electron microscope-Energy dispersive spectrometer (TEM-EDS), X-ray photoelectron spectroscopy (XPS) and Raman. The superior activation performance of CoS could be attributed to the inner-sphere complexation between CoS and sulfite and enhanced > Co(III)/>Co(II) recycling induced by reductive sulfur species via rapid electron transfer. In addition, the iohexol degradation pathways were analyzed. This study highlights the contribution of sulfur conversion in the sulfite activation process and is expected to provide a facile CoS enhanced sulfite activation method for efficient abatement of organic contaminants.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Junhao Li,Jiajie Pan,Qilan Chen,Guizheng Liu,Tong Li,Lingcai Zeng,Kai Wan,Quanbing Liu,Zhenxing Liang
It is extremely desirable to develop efficient sulfur reduction reaction (SRR) electrocatalysts for lithium-sulfur (Li–S) batteries. In this work, a small intestinal structure sulfur electrocatalyst, viz. Ni 2 P-CNTs@NHCF nanoreactor, is designed by a facile coaxial electrostatic spinning strategy. Experimental results and theoretical calculations indicate that the synergetic effect of Ni–S and Li–P dual chemical bonds between Ni 2 P and lithium polysulfides (LiPSs) optimizes the chemisorption energy of LiPSs and reduces reaction energy barriers from liquid LiPSs to solid Li 2 S, thus achieving the successive immobilization-diffusion-conversion process of sulfur species. As a result, the cell modified with Ni 2 P-CNTs@NHCF catalyst exhibits the excellent reversible capacities and cyclic stability. With the high sulfur loading of 8.13 mg cm −2 and low electrolyte/sulfur ratio of 6 μL mg −1 , it displays a significant initial areal capacity of 13.4 mAh cm −2 and remains 7.1 mAh cm −2 after 80 cycles at 0.1 C. This work offers an effective strategy on rational design of efficient electrocatalysts, and provides considerable insights into the mechanical comprehension of SRR.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Wang,Chenyang Zhou,Laihong Shen,Yuyang Long,Dongsheng Shen
Sulfur impurity in solid fuel should be paid attention to in the thermal process from the perspective of environment and sulfur recovery, especially the auto-thermal oxygen carrier aided pyrolysis/gasification (OCAP). To uncouple the complex sulfur transformation during OCAP of solid fuel and elucidate the main mechanism, several typical model compounds of various functional groups were used to investigate the kinetic analysis and sulfur transformation through temperature-programmed method. The OCAP process consisted of devolatilization and partial gasification. The activation energy of sulfur models devolatilization was less than that of partial gasification, because the required energy was much more to release lattice oxygen from oxygen carrier. Furthermore, the actual oxygen transport capacity of oxygen carrier (OC) redistributed the sulfurous gases. It was found that H 2 S was released earlier than SO 2 . H 2 S release was ascribed to the devolatilization including the reactions between radicals and hydrogen abstracted from base at low temperature (200–300 °C). The different contact modes between sulfur compounds and OC proved that S could be absorbed in the form of iron sulfide and incorporated into char at low temperature but released in the form of SO 2 by OC oxidation at the elevated temperature (400–600 °C), which was in accordance with the kinetic analysis. The migration of sulfur from disulfide had priority over that from monosulfide, and the sulfur connecting with dialkyl (benzyl) was easier to escape than that with diaryl (phenyl) in OCAP process. The fate of sulfur model compounds was conducive to reveal the complex behaviors of solid fuel with different sulfur species, and this work provides evidence to implement the desulfurization and sulfur recovery strategy.
研究领域:
化学工程
·
环境科学
·
能源技术
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Wenyan Si,Jing Gao,Yuan Gao,Fuhua Zhao,Yuan Zhang,Xiaolin Sun,Jianfei Wu
Shuttle effect of polysulfide in the cathode and the safety issues arising from dendrite formation at Li metal anode are the main challenges of traditional liquid lithium‑sulfur batteries. In order to solve the shuttle effect and prevent short circuit, the all-solid-state lithium‑sulfur battery (ASSLSB) is proposed. However, the huge volume expansion of sulfur and the improvement of sulfur conversion efficiency during charge and discharge, which could lead to the limitation of electrochemical performance. Herein, a homogeneous Ni-doped carbon-nanotubes (H-Ni-SVD@CNT) composite cathode of ASSLSB is prepared by sulfur vapor deposition to confine sulfur and promote the conversion of sulfur and Li 2 S. In this work, SVD-5-S@CNT composite cathode demonstrates high reversible discharge capacity of 1001.1 mAh g −1 after 127 cycles and capacity retention rate of 78.6 % at the rate of 0.1C and 60 °C. Moreover, H-Ni-SVD@CNT composite cathode exhibits superior electrochemical performance, displaying the discharge specific capacity of 1519.3 mAh g −1 at 0.1C and 60 °C. Meanwhile, the discharge specific capacity of H-Ni-SVD@CNT composite cathode is 1060.9 mAh g −1 at room temperature. The synergistic effect of physical confinement and chemical catalysis improves the electrochemical performance of the all-solid-state lithium‑sulfur battery. This work proposes a new strategy for the cathode structure design of the all-solid-state lithium‑sulfur battery.
研究领域:
材料科学
·
储能技术
·
电池技术
·
电化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Mengjie Zhang,Hong Xiao,Yang Liu,Wenshuo Hou,Xuting Li,Jianlin Deng,Linrui Hou,Changzhou Yuan
The sluggish redox kinetics and intrinsic dissolution of lithium polysulfides (LiPSs) critically hinder the desirable commercialization of Li-S batteries (LSBs). Purposeful modification of separators with multi-functional materials brings enormous room for both efficiently restraining the dissolution and enhancing the solid-liquid-solid conversion kinetics of LiPSs. For this, herein, hetero-architectured CoO-Co 3 O 4 hollow nanotubes (HNTs) are elaborately designed and fabricated via a self-sacrifice template methodology to modify the polypropylene (PP) separator for advanced LSBs. Besides the robust physico chemical adsorption, the endogenous CoO-Co 3 O 4 heterojunction, as authenticated by theoretical calculations and experimental verification, spontaneously creates an interfacial built-in electric field, which simultaneously enhances the active sites, accelerates the bi-directional sulfur conversion, and favors the fast electron/ion transport. Thanks to successful realization of the synergistic “electrostatic capture-energy barrier regulation-directional conversion” effect, LSBs with the hetero CoO-Co 3 O 4 HNTs modified PP separator exhibit significantly improved electrochemical performance with the long-duration cycling stability for 1000 cycles at 5 C, and a large capacity of 631.5 mAh g −1 even at a high sulfur loading (5 mg cm ‒2 ) and low electrolyte/sulfur ratio (8.0 µL mg −1 ). More essentially, our contribution here offers a viable avenue for up-and-coming hetero-catalyst functionalized separator platforms toward next-generation LSBs and beyond.
研究领域:
能源材料
·
电化学
·
纳米材料
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Tan Wang,Zhe Bai,Xiaotian Gao,Yu Bai,Yaojie Lei,Zhenhua Wang,Guoxiu Wang,Kening Sun
Single-atom catalysts (SACs) have emerged as an effective approach to improve the utilization efficiency of sulfur cathodes in lithium–sulfur (Li–S) batteries, owing to their unique atomic-scale catalytic interfaces. However, achieving fast reaction kinetics for both the liquid–solid and solid–solid conversion of lithium polysulfides (LiPSs) demands a tandem catalysis mechanism with multiple active sites, which remains a major challenge. Herein, we report the first example of an asymmetric Ta–N 5 single-atom catalyst (denoted Ta SAs/NC) with dual active sites engineered to trigger tandem catalysis and thereby promote the stepwise conversion of LiPSs. The asymmetric Ta–N 5 coordination environment induces electron redistribution, thereby intensifying d–p orbital hybridization between the Ta 5d and S 3p orbitals. In this tandem catalytic process, the Ta–S bond predominantly accelerates the liquid–solid conversion of LiPSs, whereas the N5–Li (N5 represents the fifth N atom in Ta SAs/NC) bond serves as the principal active site for the subsequent solid–solid conversion. Li–S batteries with the Ta SAs/NC interlayer exhibit a high capacity retention of 90.42 % after 500 cycles at 7 C. In addition, the cells with a high sulfur loading of 5.03 mg cm −2 deliver an exceptional initial areal capacity of 5.72 mAh cm −2 and maintain 5.01 mAh cm −2 after 30 cycles. Moreover, the pouch cell based on this interlayer exhibits excellent capacity decay of 0.21 % per cycle after 200 cycles.
研究领域:
储能
·
材料科学
·
电化学
·
催化
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2024
·
IF 24.4
Qiaowei Lin,Jiaxing Liang,Ruopian Fang,Changlong Sun,Aditya Rawal,Jun Huang,Quan-Hong Yang,Wei Lv,Da-Wei Wang
Electrocatalysts can optimize the sulfur/sulfide reaction kinetics in Li–S batteries to compete with the loss of lithium polysulfides (LiPSs) caused by the shuttling effect. However, the design rationale of electrocatalysts to drive roundtrip sulfur/sulfide conversion is lacking. Here, pairing Lewis acidic and Lewis basic active sites to reach collective adsorption of LiPSs and simultaneous activation of electrophiles and nucleophiles in LiPSs is proposed. This concept is validated by doping polyaniline with protonated metatungstate anions, which enables reduced activation energies for both sulfur reduction reaction and sulfide oxidation reaction and results in significantly improved kinetics. Such electrocatalysts enable a Li–S battery to reach a low capacity-decay rate of 0.029% per cycle for 1000 cycles. This work would offer insights into battery technologies where sulfur electrocatalysis will play pivotal roles.
研究领域:
材料科学
·
电化学
·
电池技术
·
催化
✓ 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）