INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yang Liu,Hailong Feng,Weiyi Li,Xueping Wang,Guoxiang Huang,Longxia Wang,Xingqiu Li,Yuxing Xie,Chenglu Liang
Catalysts in-situ reconstructed from transition metal sulfides for oxygen evolution reaction (OER) have been regarded as potential alternatives for the noble metal catalysts . Intriguingly, it was found that the self-optimized SO 4 2− @Cu doped Co(OH) 2 catalyst was reconstructed from bimetallic sulfide of CuCo 2 S 4 . During the OER process, the copper was partially leached and meantime doped into the in-situ generated Co(OH) 2 with SO 4 2− adsorption, while only oxides were discovered in counterparts of mono-metal sulfides. As a result, the SO 4 2− @Cu doped Co(OH) 2 catalyst exhibited superior OER performances, with low overpotentials of 211/272 mV to achieve the current densities of 10/100 mA cm −2 , exceeding the counterparts reconstructed from mono-metal sulfides. Experimental and theoretical results suggested that the in situ generated Cu doped Co(OH) 2 possessed thin and loosely layered structure with expanded lattice spacing (lattice spacing expanded from 0.28 nm to 0.46 nm) due to the SO 4 2− adsorption, making the intermediates more accessible to the active centers. In addition, the catalyst surface changed from hydrophobicity to super hydrophilicity , which greatly accelerated the mass transfer. This work indicated that the in-situ reconstruction process was greatly influenced by the interactions between metal sites and sulfide species, directly influencing the OER performances of the reconstructed catalysts.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Journal of Natural Gas Chemistry
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2012
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IF 1.348
Lincai Peng,Junping Zhuang,Lu Lin
Effects of Zr/Ti molar ratio in SO 2− 4 /ZrO 2 -TiO 2 solid acid catalyst calcined at different temperatures on its surface properties and catalytic activity were thoroughly investigated in this paper. The physicochemical characteristics of prepared samples were determined by N2 adsorptiondesorption, XRD, NH3-TPD and XPS techniques, respectively. It was found that the crystallization temperature of the samples increased after the combination of ZrO 2 and TiO 2 ; and phase transformations from the anatase to the rutile of TiO 2 species and the tetragonal to the monoclinic of ZrO 2 species were effectively suppressed at higher temperature. The sample with a Zr/Ti molar ratio of 3/1 calcined at 450 °C showed the highest surface area and the most acid sites among all the tested samples. The acid site densities of samples were relatively closed to each other if they were calcined at the same temperature, however, decreased with the calcination temperature. The result indicates that the sulfur content in samples is a crucial factor to control the acid site density. Calcining the sample at 650 °C and higher temperatures resulted in a significant desorption of sulfate ion on the samples. The synthesized samples were evaluated as a potential catalyst for glucose conversion under the near-critical methanol conditions (200 °C/4 MPa). The results suggested that the relatively weaker acid sites of the catalyst were more favorable for the accumulation of methyl glucosides, while the moderate acid sites were responsible for the formation of methyl levulinate. The catalytic activity for methyl levulinate production almost increases linearly with the catalyst acid site density. The catalyst deactivation is due to the loss of sulfate ion and the two catalysts with Zr/Ti molar ratios of 3/1 and 1/3 could effectively alleviate the deactivation caused by sulfate solution in the reaction medium and can be reused after calcination with the reuse rate of over 90% in terms of the methyl levulinate selectivity.
研究领域:
催化化学
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材料科学
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高影响因子
WATER SCIENCE AND TECHNOLOGY
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2019
·Vol. 80
·期 5
·950-960
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IF 1.624
Zhang Caiduan,Liu Feng,Wang Fengjia,Li Haotian,Zeng Fang,Ma Yongliang,Wang Lidong
In order to achieve efficient recovery of ions from the simultaneous desulfurization and denitrification wastewater, the effects of various factors (i.e. the saturation temperature, the cooling termination temperature, the stirring rate and the cooling rate) on crystallization yield, metastable zone width and crystal morphology were investigated to determine the optimal crystallization conditions of Mg 2+ //SO 4 2− , NO 3 – -H 2 O system. According to the results of experiments, the nucleation kinetics were also speculated by Nývlt self-consistent equation and classical 3D nucleation theory. Also, the crystallization products were characterized by X-ray diffraction and scanning electron microscopy. Under the determined optimal conditions, the yield of the crystal can reach 78%, and the crystal products were verified as pure MgSO 4 · 7H 2 O, whose morphology is complete without defects.
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高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xueqing Wang,Penghao Hao,Chunyan Wang,Xue Yu,Ming Tan,Jiuqing Liu,Yang Liu,Yang Zhang
To address the growing demand for high-performance membranes in sustainable water treatment, this study developed a novel nanofiltration (NF) membrane via a mixed-monomer strategy. Interfacial polymerization was conducted on macroporous polyethersulfone (PES) supports using an aqueous phase containing piperazine (PIP) and piperazine-2-carboxylic acid (PIP-COOH), and an organic phase of trimesoyl chloride (TMC). The introduction of PIP-COOH, a carboxyl-functionalized monomer, not only increased the membrane’s surface negative charge but also moderated the interfacial reaction rate, enabling the formation of a more uniform and controllable polyamide layer. By systematically adjusting the PIP/PIP-COOH ratio and monomer concentrations, the membrane structure and separation properties were fine-tuned. Under optimal conditions (3:1 PIP/PIP-COOH, 0.4 % TMC), the membrane achieved a NaCl/Na 2 SO 4 selectivity of 19.86 and a water permeance of 10.42 L·m −2 ·h −1 ·bar −1 . Additionally, outstanding antifouling performance was demonstrated, with a total fouling ratio of just 4.62 % and a flux recovery rate of 99.07 % after hydraulic cleaning. These results highlight the potential of using functionalized monomers in mixed systems to achieve a favorable balance between permeability, selectivity, and fouling resistance. The proposed approach offers a scalable and effective pathway for designing next-generation NF membranes for sustainable water treatment and resource recovery.
研究领域:
水处理技术
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膜科学
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高分子化学
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环境工程
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可持续资源回收
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DOI
高影响因子
ACS Nano
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2022
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IF 18.027
Quan Chen,Yuyang Yao,Junbin Liao,Junhua Li,Jingwen Xu,Tongtong Wang,Yuanyuan Tang,Yanqing Xu,Huimin Ruan,Jiangnan Shen
Ion-conductive polymers having a well-defined phase-separated structure show the potential application of separating mono- and bivalent ion separation. In this work, three side-chain-type poly(arylene ether sulfone)-based anion exchange membranes (AEMs) have been fabricated to investigate the effect of the stiffness of the polymer backbone within AEMs on the Cl–/NO3– and Cl–/SO42– separation performance. Our investigations via small-angle X-ray scattering (SAXS), positron annihilation, and differential scanning calorimetry (DSC) demonstrate that the as-prepared AEM with a rigid benzimidazole structure in the backbone bears subnanometer ion channels resulting from the arrangement of the rigid polymer backbone. In particular, SAXS results demonstrate that the rigid benzimidazole-containing AEM in the wet state has an ion cluster size of 0.548 nm, which is smaller than that of an AEM with alkyl segments in the backbone (0.760 nm). Thus, in the electrodialysis (ED) process, the former exhibits a superior capacity of separating Cl–/SO42– ions relative to latter. Nevertheless, the benzimidazole-containing AEM shows an inability to separate the Cl–/NO3– ions, which is possibly due to the similar ion size of the two. The higher rotational energy barrier (4.3 × 10–3 Hartree) of benzimidazole units and the smaller polymer matrix free-volume (0.636%) in the AEM significantly contribute to the construction of smaller ion channels. As a result, it is believed that the rigid benzimidazole structure of this kind is a benefit to the construction of stable subnanometer ion channels in the AEM that can selectively separate ions with different sizes.
研究领域:
材料科学
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离子分离技术
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DOI
PubMed
高影响因子
Catalysts
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2021
·Vol. 11
·期 12
·1464
·
IF 4.146
Su Yang,Xiaoxuan Guo,Xiaomei Pan,Liuyu Gu,Xueping Liu,Lijing Gao,Guomin Xiao
Concentrated sulfuric acid is generally used as a catalyst for producing brominated alkanes in traditional methods, but is highly corrosive and difficult to separate. This work reports the preparation of bromopropane from n-propanol based on a reactive distillation strategy combined with alumina-modified sulfated zirconia (Al2O3/SO42−/ZrO2) as a heterogenous catalyst. As expected, under the optimum reaction conditions (110 °C), the yield of bromopropane was 96.18% without side reactions due to the reactive distillation strategy. Meanwhile, the microscopic morphology and performance of Al2O3/SO42−/ZrO2were evaluated by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunner–Emmet–Teller (BET), Fourier transform infrared spectroscopy (FT–IR), and other characterization methods. The results confirmed that the morphology of zirconia sulfate is effectively regulated by the modification method of alumina, and more edges and angles provide more catalytic acid sites for the reaction. Furthermore, Al2O3/SO42−/ZrO2exhibited high stability and remarkable reusability due to the strong chemical bond Zr–Al–Zr. This work provides a practical method for the preparation of bromopropane and can be further extended to the preparation of other bromoalkanes.Keywords:sulfated zirconia;modification of alumina;bromopropane;catalytic distillation
研究领域:
化学工程
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催化
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有机化学
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DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2024
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IF 2
Hongxiang Xu,Wentao Li,Junfeng Wang,Jiushuai Deng,Shangqing Chen
After the NaClO solution was used to purify acetylene gas, the solution contained significant amounts of NaCl, Na2SO4, and Na2HPO4. The phase equilibrium data is the most important basic information for recovering sodium salts. In this study, the solubilities and dry-salt phase diagram for the system (Na+//Cl–-SO42–-HPO42–-H2O) were systemically studied. The dry-salt phase diagram contained one invariable point, three univariate solubility curves, and three single salt crystallization regions corresponding to NaCl, Na2SO4, and Na2HPO4·12H2O at 298.15 K and 0.1 MPa. Based on the ELEC-NRTL and Pitzer model embedded in the Aspen Plus, the phase equilibrium data for the ternary subsystem (Na+//Cl–-SO42–-H2O, Na+//Cl–-HPO42–-H2O, and Na+//SO42–-HPO42–-H2O) at 298.15 K and 0.1 MPa taken from the literature were first predicted to verify the applicability of parameters from the default database and literature. Subsequently, the models were optimized by literature solubility data, and then, the obtained parameters can well predict the phase equilibrium data for the ternary subsystem at 298.15 K and 0.1 MPa. All of these will provide basis data for the separation of sodium salt from the Na+//Cl–-SO42–-HPO42–-H2O system.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Molecular Catalysis
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2022
·
IF 5.089
Changhui Zhu,Kaiqiang Wang,Jia Luo,Baohe Tian,Jialin Sun,Xinhong Liu,Wenchao Zhu,Zhiyun Zou
α -Aromatic amino acid esters are important platform compound for drugs, sweeteners and fluorescent sensors. Due to the amphoteric dissociation and steric effect, the esterification of α -aromatic amino acids is difficult. Here, a green and efficient solid superacid, SO 4 2− -S 2 O 8 2− /SnO 2 -Nd 2 O 3 (SSSN), was synthesized and firstly used for the methyl esterification of α -aromatic L-tyrosine and L-tryptophan. The methyl esters yield was optimized with the highest L-TyrOMe yield of 93.1% and L-TrpOMe yield of 92% over SSSN-650 (SO 4 2− -S 2 O 8 2− /SnO 2 -Nd 2 O 3 calcined under 650 °C). Furthermore, it was clarified that the doping of Nd enhanced the electron-withdrawing inductive effect of SO 4 2− /S 2 O 8 2− with increased Brønsted and Lewis acidity, which were beneficial to the esterification of L-tyrosine and L-tryptophan. Besides, Nd-doping reduced the activation energy during L-Tyr esterification by kinetics study. Finally, SSSN-650 could be recycled six times with > 70% of their initial ester yield. The decrease of catalyst activity was caused by carbon deposition and species leaching. This work launched a novelty, rapid and environmental-benign technology for the esterification of α -aromatic amino acid using solid superacid.
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DOI
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Xiayi Hu,Qian Yu,Yuanyuan Cui,Juntao Huang,Elenica Shiko,Yefeng Zhou,Zhaogang Zeng,Yang Liu,Rui Zhang
The main issue for the development of CO2 capture in industry is its high energy cost. In this work, the regeneration of the chemical solvent 3-(diethylamino)propylamine (DEAPA) with or without catalyst was studied to further reduce the energy consumption. Three different catalysts (SAPO-34, MCM-41, and SO42–/TiO2) were applied into the DEAPA system to enhance the energy efficiency by lowering the heat cost per mole of CO2 released in a CO2 stripping process. The results show that solely DEAPA (without catalyst) can increase the CO2 desorption rate by 37.28%, increase the cyclic capacity by 38.02%, and reduce the heat duty by 14.85% compared to 5 M monoethanolnamine (MEA). In addition, for the catalyst–DEAPA systems, DEAPA-SAPO-34, DEAPA-MCM-41, and DEAPA-SO42–/TiO2 could lower the heat duty by 33.08%, 27.79%, and 22.41%, respectively, relative to 5 M MEA. The SAPO-34 catalyst also shows a better efficiency for increasing the CO2 desorption rate and cyclic capacity compared to the other two catalysts used. Moreover, a possible catalytic mechanism for CO2 desorption from the DEAPA–catalyst system is proposed based on the results from catalyst characterization. Through comparing the parameters of each catalyst, it can be inferred that the mesopore surface area (MSA) and the total acid sites (TAS) are the critical factors for an efficient catalyst. The combination of MAS*TAS could especially act as a key value to evaluate the performance of a catalyst for catalytic CO2 desorption.
研究领域:
化学工程
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环境科学
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催化
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DOI
高影响因子
CORROSION SCIENCE
·
2018
·
IF 4.862
Jie Qiu,Bin Leng,Huajian Liu,Digby D. Macdonald,Angjian Wu,Yanyan Jia,Wandong Xue,Guojun Yu,Xingtai Zhou
The effect of SO 4 2− on the corrosion behavior of 316 L stainless steel (SS) in molten FLiNaK (LiF-NaF-KF: 46.5–11.5–42 mol.%) salt was studied. Results reveal that the SO 4 2− in the salt remarkably accelerates the corrosion of 316 L SS by promoting the dissolution of Cr, leading to increasing intergranular corrosion of the alloy. On the other hand, the results of structural characterization indicate that the SO 4 2− can react with Mn to form MnS at the grain boundaries of the alloy. The galvanic couple between MnS and steel matrix could further accelerate the intergranular corrosion of 316 L SS in molten fluoride salt environments.
研究领域:
材料科学
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腐蚀科学
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无机化学
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核工程材料
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高温电化学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2015
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IF 1.964
Tao Wu,Jingwei Wan,Xuebing Ma
Magnetic solid acid catalysts SO 4 2− /Zr(OH) 4 –Fe 3 O 4 were prepared using magnetic Fe 3 O 4 nanoparticles , ZrOCl 2 ·8H 2 O, and sulfuric acid as starting materials in the calcination temperature range 110–650 °C. The properties of the magnetic solid acid, such as loaded SO 4 2− content, acid distribution, surface morphology, and porous structure, were characterized. In the aqueous asymmetric aldol reaction of various benzaldehydes with strong electron-withdrawing groups (R = NO 2 and CN), good to excellent catalytic performance (83%–100% yield, 86.0%–95.6% ee anti , and anti/syn = 88–96/12–4) was achieved. These nanomagnetic solid acids can be quantitatively recycled from the reaction mixture using an external magnet and reused five times without significant loss of catalytic activity.
研究领域:
化学
·
材料科学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yucai Li,Can Deng,Haotian Hu,Yida Wang,Zijian Qi,Cong Chen,Cailong Zhou,Liang Shen
Polyamide thin-film composite (PA TFC) membranes synthesized via conventional interfacial polymerization (IP) often underperform in Cl − /SO 4 2− separation due to their subpar spatial architectures. This study presents a novel strategy to fabricate advanced anion-selective nanofiltration (NF) membranes by functionalizing PA selective layer pore walls with nitrogen/oxygen-containing heterocyclic compounds (crown ether and cyclen) to tailor intrapore chemical microenvironments. Both experimental validations and molecular simulation results demonstrate that precise regulation of chemical interactions between the membrane matrix and permeation species (NaCl/Na 2 SO 4 ) enables controlled tuning of diffusion energy barriers for anions traversing the membrane. Beyond size exclusion and charge repulsion mechanisms, we employ transition state theory to elucidate the fundamental Cl − /SO 4 2− separation mechanism. The distinct roles of these compounds in modulating IP reaction kinetics and their impacts on membrane microstructure are systematically investigated. Integration of heterocycles into the PA network yields more hydrophilic, less densely packed membranes. Resultant cyclen-modified membranes achieve exceptional separation performance (water flux of 26.65 L m −2 h −1 bar −1 , Cl − /SO 4 2− selectivity of 223), while 15-crown-5-modified membranes exhibit remarkable Cl − /SO 4 2− selectivity (690, Na 2 SO 4 rejection of 99.71 %) with maintained water flux (17.50 L m −2 h −1 bar −1 ). These modified membranes also exhibit robust long-term stability and excellent fouling resistance. This work establishes a novel pathway for developing high-performance Cl − /SO 4 2− separation membranes through engineered control of ion diffusion energy barrier.
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DOI
高影响因子
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