Journal of Environmental Sciences
·
2023
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IF 6.9
Xiaoyun Chen,Guohua Jing,Bihong Lv,Zuoming Zhou
The non -aqueous solid-liquid biphasic solvent of 2-amino-2-methyl-1-propanol (AMP)/piperazine (PZ)/dipropylene glycol dimethyl ether (DME) features a high CO 2 absorption loading, favorable phase separation behavior and high regeneration efficiency. Different with the liquid-liquid phase change solvent, the reaction kinetics of CO 2 capture into solid-liquid biphasic solvent was rarely studied. In the present work, the reaction kinetics of CO 2 absorption into AMP/PZ/DME solid-liquid biphasic solvent was investigated into the double stirred kettle reactor. The absorption reaction followed a pseudo-first-order kinetic model according to the zwitterion mechanism. The overall reaction rate constant ( k ov ) and the enhancement factor ( E ) of CO 2 absorption both increased with increasing temperature. The total mass transfer resistance of the absorbent decreased with increasing temperature and increased with increasing absorption loading, so the higher reaction temperature was conducive to the absorption, and the liquid phase mass transfer resistance was the main factor affecting the absorption rate.
研究领域:
化学工程
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环境科学
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高影响因子
RSC Advances
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2025
·Vol. 15
·期 33
·26950-26958
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IF 4.6
Chunqiu Zhao,Qiang Chang,Fu Yin,Jing Li,Guowei Niu,Hulin Wang,Dan Liu,Bhekie B. Mamba,Chenghua Zhang,Alex T. Kuvarega
One-step CO hydrogenation to value-added chemicals represents a prominent yet challenging research objective for conventional catalysis processes in chemical industry. Herein, we report a rationally designed Ni-doped Zn-NC catalyst embedded within an N-doped carbon matrix for one-step CO hydrogenation to dimethyl ether (DME), demonstrating superior CO conversion compared to the pristine Zn-NC catalyst (25.9% vs. 20.6%) while both maintaining high DME selectivity (>93%). Structural characterization revealed that Ni atoms existed in a bimetallic coordination environment, which is crucial for the promoting effect of Ni. In contrast, Ni nanoparticles incorporated into Zn-NC (nanoNi–Zn-NC) reduced CO conversion to less than 17% despite retaining high DME selectivity (>92%). Besides, control catalysts containing either Ni-only or Ni/Zn nanoparticles supported on carbon support exhibited limited catalytic activity and mainly produced hydrocarbons. This work provides valuable insights into the active sites of the bimetallic Ni–Zn-NC catalysts and elucidate the structural effects of bimetallic systems for CO conversion to DME. Furthermore, this study offers a feasible framework for optimizing Zn-based bimetallic catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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能量转换
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PubMed
高影响因子
JOURNAL OF PHYSICAL CHEMISTRY B
·
2026
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IF 3.2
Jing Ma,Shuting Xu,Tianjiao Sun,Xiaokang Hu,Xinping Qiu,Zhiwu Yu
Electrolytes serve as critical components in batteries and electrolytic cells. This study proposes a framework to assess the contributions of clusters to electric conductivity. Within this framework, clusters are first identified, and their molarities are calculated by integrating excess infrared spectroscopy with density functional theory (DFT). Subsequently, the self-diffusion coefficients of these clusters are estimated through the Stokes–Einstein relation. Finally, the conductivities of charged clusters are evaluated using the Nernst–Einstein equation. By combining these steps, the percentage contribution of charged clusters to overall electric conductivity is quantitatively determined. Taking the binary system of sodium trifluoromethanesulfonate (NaOTf) and 1,2-dimethoxyethane (DME) as a model electrolyte, liquid clusters, namely, Na+(DME)3, Na+(DME)2, OTf–(DME)4, Na(OTf)2–(DME)4, (Na)2OTf+(DME)4, NaOTf(DME)2, NaOTf(DME)3, as well as DME monomer, dimer, trimer, and tetramer, were identified in the binary mixtures. Contributions from charged clusters to the overall conductivity at each experimental concentration were derived. It was found that, at low salt concentrations, Na+(DME)3 plays the dominant role, while at high concentrations, the biggest contributor is OTf–(DME)4. Together with other techniques including nuclear magnetic resonance and molecular dynamics, DME was found to interact strongly with Na+, in a mode of bidentate to make a coordination number of six. On the contrary, the interaction between DME and OTf– is weak, with negligible hydrogen bonds. The present work addresses the conductivity properties of electrolytes at the cluster level, providing physical insights into the concerned topic. It may also shed light on the design of new electrolytes to meet the needs of vigorously developing battery industries.
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高影响因子
ChemPlusChem
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2025
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IF 2.8
Chunqiu Zhao,Qiang Chang,Fu Yin,Guowei Niu,Chenghua Zhang,Dan Liu,Bhekie B. Mamba,Alex T. Kuvarega
Graphical To enhance the catalytic performance of Zn−NC in the hydrogenation of CO to dimethyl ether, highly dispersed bimetallic catalysts are synthesized through the pyrolysis different metal-doped ZIF. The incorporation of secondary metals (Mn, Fe, Co, Ni, Cu) leads to distinct variations in catalytic performance. Among them, the introduction of Cu significantly improves catalytic activity. Highly dispersed bimetallic atomic-scale catalysts have garnered significant attention in syngas conversion filed due to the synergistic effects of the precisely structured bimetallic site, which facilitate the effective activation of CO. Despite their potential, synthesizing these catalysts to meet the specific application requirements remains challenging. Herein, various bimetallic catalysts were synthesized through the pyrolysis of the bimetallic ZIF precursors which were prepared by in situ doping of different metals (Mn, Fe, Co, Ni and Cu) into the ZIF-8 structure. In the presence of a highly dispersed and highly loaded Zn, the doping content in the ultimate second metallic catalysts varied between 0.15–1.20 wt % for different metals. The catalysts were systematically characterized using XRD, BET, TEM, XPS, Raman, ICP, and H 2 -TPD techniques. Among them, the Zn−NC regulated with Cu or Ni exhibited superior catalytic performance. Notably, the Cu−Zn−NC catalyst showed the highest activity, achieving a CO conversion of 32.8 % and optimal DME selectivity approaching 95.2 % in CO hydrogenation reactions. These enhanced performance metrics were attributed to the synergetic effects of bimetallic components. The incorporation of Cu not only preserved the original Zn−N structure but also preserved the catalytic performance unchanged. This preparation strategy is expected to filter out new research targets to use in diverse catalytic applications.
研究领域:
催化化学
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材料科学
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能源化学
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PubMed
高影响因子
PHOSPHORUS SULFUR AND SILICON AND THE RELATED ELEMENTS
·
2020
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IF 1.046
Daoke Yu,Wenbin Chen,Shichao Zhang,Rakesh Chilivery,Fuhai Li,Xupeng Lu,Yibing Song,Yiwen Fang
The synthesis conditions of HZSM-5 zeolite, including crystallization temperature, crystallization time and raw material ratio, were investigated by L32 (48) orthogonal test to specifically optimize its performance in dimethyl ether (DME) aromatization for the first time. Based on the total yield of aromatic products, the synthesis conditions of HZSM-5 zeolite with the best DME aromatization properties were obtained by comprehensive analysis and validation experiments. The relationship between the aromatization performance, crystalline structure, pore structure, and acidity of HZSM-5 zeolite were analyzed. The results showed that the HZSM-5 zeolite accompanied by hierarchical structure, an appropriate Brønsted and Lewis acid content and uniform crystal morphology, was successfully synthesized under optimized conditions. Over this unmodified and un-doped catalyst, the conversion of DME approached to 99.3% and the total yield of aromatics reached was 53.5%.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Chi Sun,Yudong Xia,Xue Ye,Wenlin Xu,Hui Shi,Xinhua Gao,Jinghao Yu,Lisheng Guo,Jie Li
The direct dimethyl ether (DME) synthesis reaction via CO2 hydrogenation typically requires a bifunctional catalyst that effectively combines a methanol synthesis catalyst with a methanol dehydration catalyst, but the effect of the relationship between the two catalysts on the catalytic performance has not been as well studied. In this study, we developed a CuZnZr/Al–S(10)-PG bifunctional catalyst physically mixed with Al-modified SBA-15 and the traditional CuZnZr catalyst for the hydrogenation of CO2 to DME. A pivotal discovery is that the modulation of interaction intensity between these two constituents significantly influences the electronic configuration of each component. Through X-ray photoelectron spectroscopy characterization and methanol dehydration experiments, it was confirmed that diminishing the synergistic interplay between CuZnZr and Al-modified SBA-15, which regulated the electronic structure of the Cu–Zn interface and enhanced the Cu–Zn interfacial interaction, played a crucial role in enhancing the catalyst’s performance in CO2 hydrogenation to DME. This finding contests established beliefs about the necessity of strong synergistic interactions in such systems and provides new insights for designing rational bifunctional catalysts.
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
Journal of the Taiwan Institute of Chemical Engineers
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2026
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IF 6.9
Abrar Hussain,Ndumiso Vukile Mdlovu,Kuen-Song Lin,Chi-Jung Chang,Amin Hussain
Background The conversion of CO 2 into value-added fuels and chemicals remains one of the major challenges in catalysis and sustainable energy research. Developing efficient catalysts for CO₂ hydrogenation to methanol and dimethyl ether (DME) is essential for reducing greenhouse gas emissions and promoting carbon recycling. Methods In this work, a Zr-modified CuO–ZnO–Al₂O₃ (CZZA) catalyst was synthesized via a co-precipitation method for CO 2 hydrogenation. The catalyst systems “CZZA/HZSM-5-L” and “CZZA/com-HZSM-5” represent Zr-modified CZZA physically integrated with loofah-templated and commercial HZSM-5 (Si/Al = 25), respectively. A bio-HZSM-5 catalyst was also prepared using loofah sponge and rice husks as dual biotemplates to promote methanol dehydration into DME. The novelty lies in (i) the dual-biomass templating strategy (silica-rich rice husk vs. low-silica loofah) to achieve macro– meso –micro hierarchies while retaining MFI crystallinity, and (ii) Zr-promotion of the Cu–ZnO–Al₂O₃ matrix to enhance Cu⁺/Cu²⁺ and Cu–Zn interfacial sites, enabling efficient one-pass CO₂ → MeOH → DME conversion at 280 °C and 30 bar. Significant findings Zr incorporation significantly improved the structural and electronic properties of the CZZA catalyst, leading to enhanced surface area, active site dispersion, and CuO–ZnO interfacial synergy. Among all tested catalysts, the CZZA/HZSM-5-L bifunctional catalyst achieved the highest DME yield (13.2 %), DME selectivity (58.6 %), and CO₂ conversion (22.5 %) at 280 °C and 30 bar. An economic evaluation of 5- and 10-ton-per-day (TPD) DME production using refinery waste CO₂ showed payback periods of 2.98 and 2.44 years, respectively. Sensitivity analysis (±20 % variation in H 2 and DME prices) confirmed the payback remained below 4 years, demonstrating the technical and economic viability of the developed Power-to-DME process.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Caiyun Wang,Xingxing Wu,Yufan Xia,Xuan Zhang,Hongge Pan,Mi Yan,Yong Li,Yinzhu Jiang
Mg metal anodes experience significant passivation of harmful side reactions in conventional electrolyte consisting of magnesium bis(trifluoromethane sulfonyl)imide (Mg(TFSI) 2 ) in 1,2-dimethoxyethane (DME), which critically impedes the advancement of high-performance rechargeable magnesium batteries. Herein, an innovative electrolyte system comprising an ultra-dilute 0.02 M Mg(TFSI) 2 in DME with 4-chlorobutyl methyl ether (CME) as co-solvent is strategically devised. This unique formulation effectively suppresses the formation of TFSI − -derived passivation byproducts while simultaneously facilitating the establishment of protective Cl-rich interphase, thereby achieving exceptional reversibility in Mg plating/stripping processes. Remarkably, Mg electrodes demonstrate stable cycling performance with a minimal overpotential of 70 mV at 0.1 mA cm −2 in the optimized 0.02 M Mg(TFSI) 2 -DME/CME electrolyte. More impressively, the system maintains reversible electrochemical operation for 400 h even at 2 mA cm −2 . This work presents a novel electrolyte formulation for overcoming the limitations of Mg metal anode in conventional Mg(TFSI) 2 based electrolytes, offering new perspectives for the development of next-generation rechargeable magnesium batteries.
研究领域:
电化学
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能源材料
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电池技术
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Fanhui Meng,Lina Wang,Muhammad Asif Nawaz,Qian Wang,Zhiyuan Gong,Zhong Li
Direct conversion of syngas to light hydrocarbons has been intensively studied in recent years; however, the high selectivity of light hydrocarbons is still a challenging task to achieve a high CO conversion. Here, a bifunctional catalyst consisting of a methanol synthesis catalyst (CZA) and a methanol to dimethyl ether (DME) catalyst (Al 2 O 3 ) was employed with a hydrocarbon synthesis catalyst (SAPO-34), for syngas conversion to light hydrocarbons in a dual fixed-bed reactor. The conversion of simulated intermediates CO/CO 2 /DME/N 2 /H 2 with a molar ratio of 9/6/4/5/76, obtained from syngas conversion to DME over CZA and Al 2 O 3 , was studied over SAPO-34 zeolites. It was found that SP34-0.1 with Si/Al ratio of 0.1, exhibited low amount of strong acid (0.60 mmol/g) and high selectivity to light olefins (74.1%), while SP34-0.4 with Si/Al ratio of 0.4 exhibited high amount of strong acid (1.00 mmol/g) leading to high selectivity of light paraffins (88.4%). The in-situ DRIFTS analysis illustrated that DME can be rapidly adsorbed on the hydroxyl site of SAPO-34 and decomposed into the surface methyl species, where SP34-0.4 could produce more dimethylcyclopentenyl cationic species than SP34-0.1. It was suggested that the overall reaction route led to a high selectivity to light olefins (84.2%) with a CO conversion of 61.2% on (CZA + Al 2 O 3 ) catalyst combined with SP34-0.1, while a high selectivity to light paraffins (76.3%) could be achieved by combining with SP34-0.4 at 70.3% CO conversion. Since, the current study interprets that the selectivity of hydrocarbons can be adjusted by regulating the acidity of SAPO-34 to achieve a high CO conversion in the dual fixed-bed reactor scheme.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Jiping Ma,Shuang Li,Gege Wu,Shasha Wang,Xiaotong Guo,Liyan Wang,Xiaoyan Wang,Jinhua Li,Lingxin Chen
Novel mixed-matrix membranes (MMM) were prepared from metal-organic frameworks (MOF) (MIL-53) and poly (vinylidene fluoride) (PVDF), viz MIL-53–PVDF MMM, for the simultaneous dispersion membrane extraction (DME) of seven sulfonylurea herbicides (SUs) in aqueous environments followed by high performance liquid chromatography (HPLC) determination. The MIL-53–PVDF MMM was well characterized and major factors influencing DME performances were systematically investigated including membrane type, MOF dosage, eluent type, solution pH, extraction/elution time and salinity, etc. Under optimal conditions, the MIL-53–PVDF MMM based DME coupled with HPLC exhibited excellent linearity within 0.03–10 μg L −1 for chlorimuronethyl and 0.01–10 μg L −1 for other six SUs individual. High enrichment factor of 250 was obtained, as well as low detection limits and quantification limits ranged from 3.75 to 10.30 ng L −1 and 12.49–34.30 ng L −1 , respectively. Furthermore, the method attained high recoveries of 77.20–111.00% at three spiking levels of SUs, with relative standard deviations of 1.28–14.67% in tap water, seawater and surface water samples. Additionally, the MMM was readily separated from water and well regenerated, and could keep about 80% recovery after 25 cycles. Compared to that reported extraction materials, the MIL-53–PVDF MMM possessed the advantages of high enrichment ability, excellent reusability, good practicality and easy separation, indicating it was a promising alternative for the enrichment of SUs from aqueous environments.
研究领域:
环境科学
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分析化学
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材料科学
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Bo Fan,Wenzhi Li,Zhongkuan Luo,Xianghua Zhang,Hongli Ma,Ping Fan,Bai Xue
Using solid–liquid hybrid electrolytes is an effective strategy to overcome the large solid/solid interfacial resistance in all-solid-state batteries and the safety problems in liquid batteries. The properties of the solid/liquid electrolyte interphase layer (SLEI) are essential for the performance of solid–liquid hybrid electrolytes. In this work, the solvation reactions between Li2S–P2S5 glass-ceramic solid electrolytes (SEs) and ether electrolytes were studied, and their influence on the SLEI was examined. Although 1,2-dimethoxyethane (DME) reacted with the Li2S–P2S5 glass-ceramic SE to form a dense SLEI, 1,3-dioxolane (DOL) severely corroded the SE, resulting in a loose SLEI. Consequently, a stable SLEI formed with DME. Using a combination of the Li2S–P2S5 glass-ceramic SE and the DME-based liquid electrolyte (LE), stable lithium plating/stripping cycles over 1000 h and a hybrid Li–S battery that retained a specific capacity of 730 mAh g–1 after 200 cycles were demonstrated. The knowledge of the reactions between the sulfide electrolytes and the organic LEs is instructive for the design of stable sulfide–liquid hybrid electrolytes for advanced batteries.
研究领域:
材料科学
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电化学
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能源存储
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PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2023
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IF 9.2
Lei Zhang,Bing Sun,Qinghua Liu,Lin Song,Teibang Zhang,Xiaobo Duan
Lithium (Li) metal anode has attracted extensive research interest, while lithium dendrites and the resulting irreversible effects have restricted its development. In this study, a thin and dense solid electrolyte interface is constructed by introducing 3-(1-pyridinio)-1-propane sulfonate (PPS), a pyridine functional groups additive in DME/DOL based electrolyte to inhibit the lithium dendrite growth. The preferential decomposition of PPS has resulted in a reduction of gas generation. Subsequently, this process leads to forming of an N-rich solid electrolyte interface , which has been found to cause a decrease in polarization potential and change the behavior of lithium deposition from dendrites to a more cellular Li metal surface. As a result, our proposed electrolyte provides multiple functionalities, including remarkable rate capability, cyclic stability, and coulombic efficiency. Significantly, Li | Li symmetrical cells exhibited a stable cycle over 1200 h at a high current density and capacity of 5 mA cm −2 /15 mAh cm −2 . We are optimistic that our proposed method can be employed in future research to identify electrolytes appropriate for use in lithium metal anodes.
研究领域:
材料科学
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电化学
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能源存储
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高影响因子
危险品化学品经营许可证（带存储）