CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Ying Fang,Baoyu Qian,Ying Yang,Yang Song,Zhaoguang Yang,Haipu Li
Purification of high-arsenic (>10 µg/L) groundwater is of significance for drinking water safety all around the world. Considering the dominant presence of arsenite (As(III)) in groundwater and ineffective adsorption of As(III) by traditional adsorbents, the magnetic Zn/Co bimetallic MOFs (Zn/Co MOFs) which contain both catalytic and adsorption sites were prepared, and coupled with peroxymonosulfate (PMS) to realize the efficient simultaneous oxidation of As(III) and adsorption of evolved As(V). Considering the vital roles of oxidation and adsorption, the molar ratio of Zn and Co precursors was tuned ranging from 1: 1 to 9: 1 during Zn/Co MOFs synthesis to balance the catalysis and adsorption processes in the heterogeneous PMS system for As(III) immobilization. It was found that Zn/Co MOFs with Zn and Co molar ratio of 5: 1 possessing moderate catalytic performance and best adsorption capacity outperformed removal performance for As(III). The presence of PMS significantly promoted the elimination of both As(III) (the initial adsorption rate increased from 31.19 to 358.96 µg/g/min) and As(V) (the initial adsorption rate increased from 354.12 to 497.85 µg/g/min), which not only oxidized As(III) into As(V) by reactive species generated from PMS activation but also provided additional adsorption sites through enlarging pore size and changing chemical environment. Furthermore, Zn/Co MOFs coupled with the PMS system exhibited outstanding reusability and effectiveness for remediation of real high-arsenic groundwater.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2017
·
IF 3.752
Tiantian Cao,Zijian Zhou,Qian Chen,Zhen Li,Shengming Xu,Jianlong Wang,Minghou Xu,Teresa Bisson,Zhenghe Xu
A novel class of magnetically responsive catalytic sorbents are proposed and synthesized with a potential application to simultaneous removal of Hg 0 and NO at low temperature from the flue gases of coal-fired power plants. The catalytic sorbent consists of magnetite (Fe 3 O 4 ), molecular sieve (HZSM-5), supported silver nanoparticles and catalytically reactive component of V 2 O 5 . Each of these materials provides a unique function for the purpose of capturing mercury, removing NO, and separation from fly ash. After separation from the fly ash, the spent sorbent can be regenerated and reused, leaving an uncontaminated fly ash product. The successful synthesis as designed was confirmed and properties of the catalytic sorbent were characterized by several methods. The synthesized catalytic sorbent was able to completely capture Hg 0 at 150 °C with a capture capacity as high as 32.4 μg·g −1 , while achieving 84% removal of NO at 150 °C. Even at a relatively high space velocity, the catalytic sorbent achieved 97% Hg 0 and 80% NO removal simultaneously, while maintaining a good stability after repetitive regeneration and recycle. The magnetically responsive catalytic composite was shown to be a promising candidate for multi-pollutant emission control from coal-fired power plants.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2018
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IF 4.908
Xin Li,Yilin Xu,Chen Zhang,Hong Wang,Yongji Song,Wei Zhang,Cuiqing Li
Photocatalytic-adsorptive desulfurization of model fuel by the H 2 O 2 -assisted synthesized TiO 2 -SiO 2 (TiO 2 -SiO 2 -H) was investigated using air as the oxidant under UV irradiation. TiO 2 -SiO 2 -H was synthesized hydrothermally in the presence of H 2 O 2 and characterized by scanning electron microscopy (SEM), N 2 adsorption, X-ray diffraction (XRD), UV–vis diffuse reflectance spectroscopy (UV–vis DRS) and photoluminescence spectrum (PL). Compared to TiO 2 -SiO 2 synthesized in the absence of H 2 O 2 , Ti 0.25 SiO y -H showed greatly enhanced photocatalytic-adsorptive desulfurization performance due to its increased surface area, greatly increased UV absorption and decreased recombination of photogenerated hole/electron pairs. The Ti/Si molar ratio was optimized to 0.3 with the sulfur removal of 100% after reaction for 1 h at the fuel-to-Ti 0.3 SiO y -H weight ratio of 20, and the sulfur content could still be reduced to be <1 ppmw when the fuel-to-Ti 0.3 SiO y -H weight ratio was increased to 80. Moreover, TiO 2 -SiO 2 -H based photocatalytic-adsorptive process bears high selectivity for removing organosulfur in the toluene-containing fuel. The sulfur removal for model fuel containing 25 wt% toluene could reach 98.4% after reaction for 5 h. The photocatalytic-adsorptive selectivity of Ti 0.3 SiO y -H for organosulfur compounds in model diesel fuels followed the order of dibenzothiophene > 4,6-dimethyldibenzothiophene > benzothiophene. The desulfurization performance of TiO 2 -SiO 2 -H was basically stable after four consecutive desulfurization-regeneration cycles.
研究领域:
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
FUEL
·
2016
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IF 3.611
Xiaoling Ren,Guang Miao,Zhiyong Xiao,Feiyan Ye,Zhong Li,Haihui Wang,Jing Xiao
This study investigates catalytic adsorptive desulfurization (CADS) of model diesel fuel using TiO 2 /SBA-15 under mild conditions. The TiO 2 /SBA-15 was prepared by a facile incipient wetness impregnation method and characterized by N 2 adsorption and X-ray diffraction. The CADS referred to ADS performance were evaluated in a batch reactor. High desulfurization uptake of 12.7 mg/g was achieved at low sulfur concentration of 15 ppmw-S by TiO 2 /SBA-15 under CADS, which was two-magnitude higher than that under ADS without the in-situ catalytic oxidation of dibenzothiophene. Kinetic results suggested that the CADS equilibrium over TiO 2 /SBA-15 was reached fast in 0.5 h. In the CADS–TiO 2 /SBA-15 system, the TiO 2 loading, cumene hydroperoxide/dibenzothiophene ratio and CADS temperature were optimized to be 10 wt%, 2, and 35 °C, respectively. Furthermore, desulfurization tests in 5 consecutive CADS-regeneration cycles suggested that the bi-functional TiO 2 /SBA-15 can be regenerated by acetonitrile washing followed with oxidative air treatment. The CADS–TiO 2 /SBA-15 mechanism went through the oxidation of DBT to oxidized DBTO 2 over TiO 2 /SBA-15 by cumene hydroperoxide, which was followed by the adsorption of the oxidized DBTO 2 over TiO 2 /SBA-15. The superior desulfurization uptake at low sulfur concentration range, fast adsorption kinetics, excellent regenerability, operation at mild conditions, and facile and low-cost adsorbent synthesis make the CADS–TiO 2 /SBA-15 system an effective and economic desulfurization approach for ultra-clean fuel production.
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
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
·
IF 3.171
Cuiting Yang,Bowen Wu,Zewei Liu,Guang Miao,Qibin Xia,Zhong Li,Michael J. Janik,Guoqing Li,Jing Xiao
Ultra-deep desulfurization of transformer oil is of great demand among power industry. In this work, the effective and deep removal of various types of organosulfurs, including mercaptan, sulfide and disulfide via catalytic adsorptive desulfurization (CADS) using bifunctional Ti-based adsorbent is reported. Compared to adsorptive desulfurization (ADS), dramatically improvement of the organosulfur uptakes were achieved under CADS process. The equilibrium adsorption capacity at 5 μg∙g −1 S reached up to 15.7, 33.4, 11.6 and 11.9 mg∙g −1 for propyl mercaptan( n -PM), dimethyl sulfide(DMS), di- t -butyl disulfide (DTBDS) and dibenzyl disulfide (DBDS), which was 262, 477, 97 and 128 times to that of ADS process, respectively, and was the highest among the reported desulfurization adsorbents. Moreover, it achieved superior breakthrough capacity of 2050, 530 and 210 ml F·(g A) −1 at the breakthrough S concentration of 1 μg∙g −1 of the commercial transformer oil S containing 10, 50 and 150 μg∙g −1 , respectively. The effectiveness of CADS is associated to the transformation of sulfur species to higher polar sulfonic species with the assistance of mild oxidant, which can be readily captured by silanol groups on SiO 2 through H-bonding interaction. The excellent recyclability of the adsorbent can be realized through solvent washing or oxidative air treatment. This work provides an effective and economic approach for the elimination of trace amount of mercaptan, sulfide and disulfide from transformer oil.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
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2013
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IF 3.777
Ruizhuo Ouyang,Wangyao Zhang,Shilin Zhou,Zi-Ling Xue,Lina Xu,Yingying Gu,Yuqing Miao
We report here the successful fabrication of an improved Bi film wrapped single walled carbon nanotubes modified glassy carbon electrode (Bi/SWNTs/GCE) as a highly sensitive platform for ultratrace Cr(VI) detection through catalytic adsorptive cathodic stripping voltammetry (AdCSV). The introduction of negatively charged SWNTs extraordinarily decreased the size of Bi particles to nanoscale due to electrostatic interaction which made Bi(III) cations easily attracted onto the surface of SWNTs in good order, leading to higher quality of Bi film deposition. The obtained Bi/SWNTs composite was well characterized with electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM), the static water contact angle and the voltammetric measurements. The results demonstrate the improvements in the quality of Bi film deposited on the surface of SWNTs such as faster speed of electron transfer, more uniform and smoother morphology, better hydrophilicity and higher stripping signal. Using diethylene triaminepentaacetic acid (DTPA) as complexing ligand, the fabricated electrode displays a well-defined and highly sensitive peak for the reduction of Cr(III)–DTPA complex at −1.06 V (vs. Ag/AgCl) with a linear concentration range of 0–25 nM and a fairly low detection limit of 0.036 nM. No interference was found in the presence of coexisting ions, and good recoveries were achieved for the analysis of a river sample. In comparison to previous approaches using Bi film modified GCE, the newly designed electrode exhibits better reproducibility and repeatability toward aqueous detection of trace Cr(VI) and appears to be very promising as the basis of a highly sensitive and selective voltammetric procedure for Cr(VI) detection at trace level in real samples.
研究领域:
分析化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Hui Wang,Wangsheng Yu,Xu Peng,Zewen Chen,Shengji Wu,Qinqin Yu,Wei Yang,Jie Zhou
In the present work, highly efficient catalytic adsorbents for Hg 0 removal in both oxygen-rich and deficient atmosphere are developed based on an “adaption” strategy. Firstly, a series of simplified SiO 2 -based catalytic adsorbents are prepared as model catalysts to gain a deeper insight into the mechanism of the catalytic Hg 0 removal process. It is found that for the effective Hg 0 removal, the catalytic adsorbent should possess an “assembling” structure involving both Hg 0 and oxygen activation sites. An “adaption” strategy is thus implemented for the devise of the catalytic adsorbent, including the functional adaption of different active sites for the reactants and the synergistic function of different active sites. Accordingly, high-efficiency catalytic adsorbent with strong redox property is developed for oxygen-rich atmosphere, while the catalytic adsorbent with high oxygen storage/release property is developed for oxygen-deficient conditions. Moreover, regeneration investigation indicates that the activities of spent catalytic adsorbents are almost fully recovered through the temperature programmed decomposition and desorption (TPDD) process. It is believed that the present “adaption” strategy for catalyst design has guiding significance for the rational and controllable construction of catalysts for other catalytic processes.
研究领域:
环境催化
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大气污染控制
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材料化学
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表面科学
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化学工程
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环境功能材料
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Ran Liu,Chang Wang,Jingran Yang,Chen Liu,Liberty Mguni,Xinying Liu,Yali Yao,Fatang Li
There is a challenge with designing catalysts that simultaneously possess active sites for catalyzing the generation of reactive oxygen species (ROSs) and effectively overcoming mass transfer resistance in oil–water biphasic systems. In this study, a novel, highly efficient oxidative desulfurization (ODS) strategy is proposed that uses an ILs-loaded metal–organic framework (MOF) coupled material as a catalyst. The IL@MOF ([Hnmp]HSO 4 @MIL-125(Ti)) coupled material prepared by loading [Hnmp]HSO 4 onto MIL-125(Ti) has catalytic-adsorption synergistic capability. It demonstrated outstanding oxidative desulfurization performance by achieving nearly a 100 % removal of dibenzothiophene (DBT) from model oil with a dosage of 0.04 g IL@MOF per 10 mL of model fuel under mild conditions (50 °C, 10 min). By comparing the experimental results with the characterization data, it is suggested that [Hnmp]HSO 4 @MIL-125(Ti) converts superoxide radicals (•O 2 − ) into 1 O 2 through oxygen vacancies (Ov) and that the catalytic action of Ti on the oxidation of DBT is primarily based on a 1 O 2 -driven non-free radical mechanism. [Hnmp]HSO 4 @MIL-125(Ti) serves as a favorable medium for contact to be made between ROSs and sulfides, which indicates an efficient catalytic-adsorption synergy.
研究领域:
环境科学
·
材料化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chaojie Li,Yan Zhao,Yongguang Zhang,Dan Luo,Jiabing Liu,Tong Wang,Wanjie Gao,Haipeng Li,Xin Wang
Lithium-sulfur (Li-S) batteries have been long deemed as next generation power supply for portable electronic and vehicle application due to their extremely high theoretical energy and power density. However, the shuttle effect of soluble lithium polysulfides (LiPs) and sluggish Li-S chemistry has severely limited their wide implication. Herein, we designed an ultrathin and vacancy-rich ZnCo-layered double hydroxide (ZnCo-LDH) anchored on CNT substrate (noted as CNT-LDH/Ar). Theoretical calculations and analysis at the experimental level are used to comprehensively explain the mechanism by which the oxygen vacancies (Vo) regulate the catalytic activity and adsorption capacity mechanism. The introduction of CNT not only improves a three-dimensional conductive network, but also exposes more active sites for polysulfide adsorption and conversion. More importantly, our design of Vo endows the material with excellent half-metallicity properties, adsorption capacity and low redox barrier. Benefiting from these properties, the S/CNT-LDH/Ar cathode exhibited excellent rate capability with 524.3 mAh g −1 at 5 C, and maintained an excellent cyclability over 500 cycles at 1.0 C with a capacity fading of only 0.042% per cycle. Most importantly, decent cyclability can be acquired with a remarkably raised sulfur loading up to 5.5 mg cm −2 with the lean electrolyte/sulfur (E/S) ratio of 6 mL g −1 .
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Zhujun Huang,Zhan Lai,Dongying Zhu,Haiyan Wang,Chenxi Zhao,Guihua Ruan,Fuyou Du
The electrospun graphene oxide/MIL-101(Fe)/poly(acrylonitrile- co -maleic acid) nanofibers (E-spun GO/MIL-101(Fe)/PANCMA NFs) were fabricated by a facile electrospinning method and used as integrated photocatalytic adsorbents (IPAs) to remove dye pollutant from water samples. Compared with E-spun GO/PANCMA and E-spun MIL-101(Fe)/PANCMA NFs, the fabricated E-spun GO/MIL-101(Fe)/PANCMA NFs exhibited higher adsorption ability and excellent photocatalytic activity towards a model pollutant Rhodamine B (RhB). Under the optimized conditions, the as-prepared IPAs achieved almost complete adsorption of RhB within 15 min with the maximum adsorption capacity of 10.46 mg/g. Under visible-light irradiation, 93.7% of RhB in 20 mL water sample was degraded within 20 min, and the degradation kinetics of RhB fitted well with the first-order kinetic model. In addition, LC-MS analysis of the RhB degradation products confirmed the degradation pathways, and the generated •OH radicals played important roles in the degradation process. Importantly, the E-spun GO/MIL-101(Fe)/PANCMA NFs exhibited good reusability and could be reused for consecutive 20 cycles, which make them promising candidate materials in the field of industrial applications and environmental remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Runlong Hao,Zhen Qian,Xiaojie Yang,Mengchao Luo,Xiaohe Feng,Wanting Qiao,Yi Zhao,Bo Yuan
Developing efficient catalysis-adsorption method for elemental mercury (Hg 0 ) removal with wide temperature window and good sulfur/water resistance is a hot topic. In this study, a novel method of microwave (MW) catalysis of MnO 2 modified molecular sieve (Mn@MOS) composite for Hg 0 removal was developed. Results indicated that Hg 0 removal efficiency of MOS was poor, only 18% at 150 °C, while the efficiency was significantly increased to 97.8% when MW/Mn@MOS was used. Compared with thermo-catalysis way, MW irradiation method achieved better Hg 0 removal efficiency (97.8% vs 86.4%) under a wider temperature window (150–450 °C), and sulfur/water resistance were greatly strengthened under MW irradiation. The dynamical adsorption capacity of Hg 0 was calculated as 1.52 mg/g when the efficiency was below 80%. Kinetic analysis indicated that MW field significantly increased the rate constant and reduced the activation energy. The fate of Hg 0 was unfolded: almost 96% of Hg 0 was chemisorbed as HgO, less than 4% was converted to gaseous Hg 2+ . The mechanism was speculated as followed: (i) excited active site of *MnO 2 was first generated under MW irradiation; (ii) then the oxidizing species including Mn(IV)/Mn(III), O ads , O latt and O* dominated the Hg 0 removal process; (iii) the reactive oxygen species of O ads , O latt and O* were replenished by the interaction between oxygen vacancies and free O 2 . This study first demonstrates the superiority of MW catalysis towards Hg 0 removal, and provides a new thought on the development of the novel Hg 0 removal technologies .
研究领域:
环境科学
·
催化
·
污染控制
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）