MACROMOLECULES
·
2019
·
IF 5.997
Cheng-Jian Zhang,Xing-Hong Zhang
Utilization of carbon disulfide (CS2), a low-cost and sulfur-rich one-carbon (C1) feedstock, for making sulfur-containing polymers is important for both polymer chemistry and applied environmental science. However, the production of well-defined sulfur-containing polymers from CS2 and epoxides remains a key challenge. Here, we report a robust coupling reaction of CS2 and epoxides for chemoselectively producing poly(thioether)s and carbonyl sulfide (COS) in one pot. The resultant polymer has exclusive thioether units and a thiol (−SH) terminal. This route takes advantage of oxygen/sulfur exchanges through two consecutive reactions, i.e., cycloaddition of CS2 to epoxides and dethiocarboxylative ring-opening polymerization of the generated cyclic dithiocarbonates. The process can be conducted in ambient air with several commercially available organic bases as catalysts (initiators) and extended to a variety of epoxides, yielding COS and diverse poly(thioether)s with tens of grams. This work furnishes an original and practical strategy for utilizing CS2 as a sulfur feedstock in polymer synthesis.
研究领域:
高分子化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Mengmeng Shao,Yangfan Shao,Shengjie Ding,Rui Tong,Xiongwei Zhong,Lingmin Yao,Weng Fai Ip,Baomin Xu,Xing-Qiang Shi,Yi-Yang Sun,Xuesen Wang,Hui Pan
Searching photocatalysts for efficient hydrogen production has been a challenging issue for solar-energy harvesting. Using co-catalyst is proven to be an effective approach to improve the efficiency of photocatalyst in water-splitting. Here, we report that carbonized MoS2 (MoS2/Mo2C) can be a superactive co-catalyst in solar-driven hydrogen production. We show that MoS2/Mo2C decorated CdS achieves a high photocatalytic hydrogen evolution rate (34 mmol/h/g, ∼112 times higher than pure CdS) and excellent apparent quantum efficiency (41.4% at 420 nm). The outstanding photocatalytic performance of MoS2/Mo2C/CdS is attributed to the metallic characteristic of MoS2/Mo2C and suitable Gibbs free energy of hydrogen adsorption, leading to enhanced light absorption, fast separation and transportation of photoinduced carriers, and optimal activity in hydrogen evolution reaction (HER). We further show that MoS2/Mo2C as co-catalyst can also dramatically improve the photocatalytic activity of g-C3N4. Our findings demonstrate that the carbonized transition metal disulfide can be active as co-catalyst in photocatalysis, providing guidance on exploring novel photocatalysts for energy harvesting.
研究领域:
材料科学
·
能源科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jiaxin Qu,Xueqian Wang,Langlang Wang,Bowen Xu,Ping Ning,Yixing Ma,Yibing Xie,Rui Cao,Qiang Ma
A nonmetallic N-doped Zr/Ti-based catalyst was prepared to investigate the effect of N addition on catalytic performance for carbon disulfide (CS 2 ) hydrolysis. The characterization of the catalyst indicated that doped N atoms were present as interstitial N in the TiO 2 lattice, resulting in an increase in the number of basic sites of the catalyst from 1.64 to 2.37 and from 0.68 to 2.53 for weakly basic and strongly basic sites, respectively. In addition, the doping of N promoted the formation of OH groups, which were favorable for the hydrolysis of CS 2 , from water (H 2 O) adsorbed on the catalyst, thus greatly improving the performance of catalytic CS 2 hydrolysis. However, N doping reduced the amount of chemisorbed oxygen on the catalyst surface from 44.7% to 33.4%, thus decreasing the oxidation reaction of the hydrolysis product H 2 S and improving the stability of the catalyst. CS 2 hydrolysis reaction activity and catalyst lifetime were tested. The experimental results demonstrated that the catalytic CS 2 hydrolysis performance was greatly improved after N doping, and the temperature to obtain 100% conversion was reduced from 180 °C to 130 °C. Selectivity to H 2 S was greatly improved with N-doped catalysts. Furthermore, the resistance of the catalyst to sulfate was improved. Nonmetallic N-doped Zr/Ti-based catalysts offer a new strategy for blast furnace gas desulfurization.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Hao Zhou,Zhe Hong,Lijiao Ma,Yingyuan Tan,Jingcheng Xu,Wenzhi Jia,Junhui Li
The experiments of the adsorption removal of CS 2 impurity from a mimetic coke oven gas were performed by using a series of Na-type zeolites as adsorbents. Combining with the diffusion & simulation calculations and several characterizations, it's found both the development degree and the diffusion ability of microporous systems significantly influence the adsorption performance of these Na-type zeolites on which the physical absorption was predominant for CS 2 molecules. Firstly, compared with NaZSM-5 or NaSAPO-34, the NaY with FAU-type framework exhibited a much higher breakthrough adsorption capacity, primarily due to its much higher microporous surface area & volume and larger-size channels, which ensured a broader adsorption space, a high-efficiency molecule-diffusion and a high adsorption utilization of micropores. Secondly, alkali-treatment introduced some mesopores into NaZSM-5 crystals but also resulted in a declined integrity of microporous structure, causing an obvious decline of adsorption performance. Thirdly, the nano-crystal NaZSM-5 or NaY exhibited a much higher breakthrough adsorption capacity than that of the corresponding micron-crystal zeolite, primarily attributed to both the increased microporous surface area & volume and the shortened micropore diffusion-path length of the former. In addition, a breakthrough adsorption capacity of up to 0.251 g/g was obtained in the first adsorption use of a nano-NaY-0.909 sample at 298 K, and it's 0.229 g/g in even the sixteenth time of operation (by then, total adsorption service hours were 80.58 h). Our work may provide an important reference for developing high-performance adsorbents for removing gaseous CS 2 impurity in coke oven gas.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Ruoyu Dai,Xipao Chen,Yaoping Hu
Trace level of CS 2 in water causes a serious threat to the environment and living organisms. Thus, the development of reliable methods for its sensitive detection is quite necessary. Herein, we design a dual-emission platform composed of blue and yellow emissive carbon dots (B-CDs and Y-CDs) for ratiometric fluorescence determination of CS 2 . B-CDs, serving as the indicator, are functionalized by hydrophilic polyethylenimine groups on the surface, which can react with CS 2 to produce hydrophobic dithiocarbamate moieties, resulting in the aggregation of nanoparticles and quenching of blue fluorescence. In contrast, Y-CDs without polyethylenimine groups exhibit no reactivity toward CS 2 and act as the internal reference. With the increase of CS 2 concentration, the blue fluorescence of the sensing platform at 461 nm continually drops, but the yellow fluorescence at 560 nm keeps nearly constant. Correspondingly, the vivid color change from blue-white to yellow can be observed by the naked eyes, realizing the visual detection. There is a linear relationship between the fluorescence intensity ratio (I 461 /I 560 ) and CS 2 concentration in the range of 7.7–1400 μM. The detection limit is as low as 2.3 μM. Furthermore, the sensing platform is successfully applied to monitor CS 2 in real water, validating its good practicability.
研究领域:
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN POLYMER JOURNAL
·
2022
·
IF 5.546
Yejun Luo,Zheng Li,Yufang Chen,Tao Jin
Hydrophobic modification of cellulose via activation synergistic activators regenerated by electron transfer (ARGET) atom transfer radical polymerization (ATRP) method has been proved to effectively improve the long-term hydrophobic stability of cotton filter fabric. However, the extra activation process will inevitably increase the complexity of the reaction process. In this work, carbon disulfide (CS 2 ) was incorporated into the ARGET-ATRP reaction system to avoid adding redundant reaction links. Specifically, the activation and acyl bromination processes were combined, and then the graft modification reaction between the acyl bromide cotton filter fabric and 1-octadecene (1-Oct) was realized by the ARGET-ATRP. The effect of the combined process on the hydrophobic modification reaction and performance of cotton filter fabric was investigated. The results showed that, under the optimum dosages of activator CS 2 , acyl bromide reagent BiB and monomer 1-Oct, the activator CS 2 was directly incorporated into the acyl bromination process. And after ARGET-ATRP Hydrophobic modification, the initial water contact angle (CA) of the obtained hydrophobically modified cotton filter fabric reached 145.0°, the residual contact angle (RCA) after the water droplet retention time of 210 min could still arrive at 125.4°, showing a corresponding attenuation rate (Dr) of 13.5%, which suggested excellent hydrophobicity and durability. Notably, the hydrophobically modified cotton filter fabric also exhibited excellent resistance to chemical corrosion, abrasion resistance and ultrasonic stripping resistance. Furthermore, this hydrophobically modified filter fabric can efficiently separate different types of oil–water mixtures. Even after 12 cycles of oil–water separation process, the separation efficiency still exceeded 95%, and the CA of the modified filter fabric before and after separation was basically unchanged.
研究领域:
材料科学
·
纺织工程
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Yuxuan Xie,Zhao Li,Ziruo Zeng,Lina Sun,Shuangyou Bao,Xin Sun,Kunlin Li,Chi Wang,Fei Wang,Ping Ning,Kai Li
To investigate the mechanism of the role of active center size on the selectivity of methyl mercaptan (CH 3 SH) and methane (CH 4 ) in the deep hydrogenation reaction of carbon disulfide (CS 2 ), it was first derived from DFT calculations that the Pt cluster geometries showed a decreasing and increasing pattern on the energy barriers of the two key hydrogenation steps: (I) HCSS* to HCSSH* and (II) deep hydrogenation of CH 2 S* to CH 3 SH. For further validation, we synthesized Pt NPs with varied average sizes (1.7–4.0 nm) using a reduction-agglomeration strategy to probe the source of size sensitivity at low Pt loading. It was found that the active centers of Pt NPs located in the 2.0–3.0 nm region have the highest proportion of medium-coordinated Pt sites, which can effectively promote hydrogen spillover and enhance the HCSS* pathway. Finally, with this modulation strategy, the catalytic activity and selectivity were significantly improved at 1 wt% Pt loading, which exceeded that of the fresh 4 wt% Pt/Al 2 O 3 catalyst, and the long-term stable production of CH 3 SH (selectivity was maintained at 80 %) was achieved at 250 ℃ in the high-concentration CS 2 environment.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2022
·Vol. 119
·期 22
·e2202449119
·
IF 12.779
Qiliang Chen,Wenmin Wang,Xin Li,Wei Guo,Yongzhu Fu
Organodisulfides (RSSR) are a class of promising active materials for redox flow batteries (RFBs). However, their sluggish kinetics and poor cyclic stability remain a formidable challenge. Here, we propose carbon disulfide (CS2) as a unique redox mediator involving reversible C-S bond formation/breakage to facilitate the reduction reaction of organodisulfides in RFBs. In the discharge of RSSR, CS2 interacts with the negatively charged RSSR-• to promote cleavage of the S-S bond by reducing about one-third of the energy barrier, forming RSCS2Li. In the recharge, CS2 is unbonded from RSCS2Li while RSSR is regenerated. Meanwhile, the redox mediator can also be inserted into the molecular structure of RSSR to form RSCS2SR/RSCS2CS2SR, and these new active materials with lower energy barriers can further accelerate the reaction kinetics of RSSR. With CS2, phenyl disulfide exhibits an exceptional rate capability and cyclability of 500 cycles. An average energy efficiency of >90% is achieved. This strategy provides a unique redox-mediating pathway involving C-S bond formation/breakage with the active species, which is different from those used in lithium-oxygen or other batteries.
研究领域:
电化学
·
材料科学
·
能源存储技术
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）