INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Dezhu Zhang,Su Fan,Kenan Xu,Haotian Liu,Nana Chang,Yijie Wang,Yixing Wang,Kang Huang,Zhi Xu
Vanadium flow battery (VFB) shows great potential in balancing the volatility of renewable energy. In this work, we investigated, for the first time, the various properties of crystalline ZSM-5 membranes prepared through the organic template-free gel strategy in VFB. The subnano windows (∼0.55 nm) of ZSM-5 zeolite provided selective transport paths for protons (∼0.27 nm) and blocked the vanadium (>0.6 nm) migration through pore repulsion effect. The zeolite membranes exhibited a very low vanadium penetration rate (0.05 mmol L–1 h–1), achieving a Coulombic efficiency (CE) of 96.1%, a voltage efficiency of 78.3%, and an energy efficiency of 75.3% at the current density of 40 mA cm–2. Notably, ZSM-5 prepared using the template-free strategy eliminates the need for a high-temperature calcination step, and the membrane has a lower defect density and exhibits a higher CE. The self-discharge time of the ZSM-5 zeolite membrane increased up to 78 h. Furthermore, the charge–discharge performance kept stable more than 300 cycles at 60 mA cm–2.
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Environmental Chemistry
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2024
·Vol. 20
·期 7
·292-301
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IF 2
Xiao-Yan Cao,Min Liu,Ling Li,Gui-Peng Yang
Environmental context Organophosphorus (OP) is bioavailable to phytoplankton with photolysis can play an important role in the process. The photolysis behaviour of an OP (adenosine 5′-monophosphate, AMP) in seawater was investigated, and AMP can release inorganic phosphate under environmentally relevant light conditions, indicating OP photodegradation might be important in the phosphorus biogeochemical cycle. The results are helpful to further understand the bioavailability and cycle of OP in marine environment.Rationale Organic phosphorus (OP) is a potential source of bioavailable phosphorus for phytoplankton through photolysis and other degradation processes. Therefore, OP photodegradation plays an important role in phosphorus biogeochemical cycle.Methodology Taking adenosine 5′-monophosphate (AMP) as a model OP, we investigated the photolysis behaviour in seawater and discussed the mechanism. The photolysis dynamics were studied based on the inorganic phosphorus production at appropriate time intervals, which was analysed by spectrophotometric molybdenum blue method. The effects of medium, light and radicals were investigated.Results It was found that AMP can release inorganic phosphate under photosynthetically active radiation and ultraviolet (UV) with UVB being the most reactive band. The degradation of AMP in seawater was lower than that in deionised water under the same conditions, and the fresh seawater was more beneficial than aged seawater. The kinetics could be described by apseudo-first order equation. Fe3+ can promote the photolysis due to the generation of ·OH radicals, while within the range of this study, changes of Fe3+ content have no substantial effect on the promotion. The influence of ethanol and tetrahydrofuran as radical inhibitor showed evident inhabitation to the degradation, indicating that ·OH and 1O2 played an important role in the process, and ·OH seemed more important than 1O2.Discussion OP photodegradation is of importance in the phosphorus biogeochemical cycle. Varying properties of the medium and light can affect the OP transformation in seawater. The results are helpful to further understand the bioavailability and cycle of OP in the marine environment.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Chunxiao Gong,Zhaoyang Ju,Qixuan Lin,Xianqing Lv,Richard Lee Smith,Lujiang Xu,Yang Cao,Li Shuai,Zhen Fang
Cellulose acetate (CA) is a versatile biopolymer derivative widely used in consumer products such as cigarette filters, textiles, and plastics. The extensive use of CA-based products generates substantial plastic waste, which can persist in the environment for over a decade due to its low biodegradability, posing serious environmental challenges. Herein, we report a one-step conversion process that transforms CA plastic waste into 5-hydroxymethylfurfural (HMF) while simultaneously recovering acetic acid. By employing AlCl 3 as a catalyst in an acetone-water solvent system at 160°C for 50 min, CA exhibited a 53.7 % HMF yield, a threefold increase compared to untreated cellulose, while also achieving a 97.3 % theoretical yield of acetic acid. The HMF yield exceeded 50 % when cigarette filters or CA fabrics were used as substrates. Molecular dynamics simulations revealed that the acetyl groups in CA enhance its coordination with acetone molecules, reducing the probability of protonation at the C1 and C4 oxygen atoms of the CA monomer and thereby suppressing the formation of undesired byproducts. Furthermore, the in-situ regenerated acetic acid actively promotes the HMF production. This study establishes a viable pathway for upcycling CA waste while advancing sustainable management strategies for CA-based plastics, offering a promising solution to mitigate environmental impacts.
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Nanomaterials
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2025
·Vol. 15
·期 9
·639
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IF 4.3
Mingbo Guo,Yijun Wang,Lei Zhang,Junran Lu,Chang Gong,Wanning Zhang,Yuxi Fang,Xinyuan Zhu,Shunai Che
Zeolite is increasingly recognized for its enhancement of low-frequency acoustic performance in microspeakers. The aging characteristics of zeolite have been regarded as the critical factor for the commercial viability of mobile phones products, but the mechanism remains ambiguous. Here, the low-frequency acoustic performance of hierarchically structured ZSM-5 was investigated through aging with water and acetic acid (AA). It was discovered that water vapor augmented the resonance offset as it enhanced the structure of the zeolite, resulting in a lower water content. The resonance offset of ZSM-5 significantly decreased after the adsorption of AA vapor, as excessive AA was adsorbed through both physical and chemical adsorption, causing partial destruction of supermicropore and mesopores. The performance of ZMS-5 stored with vapor of AA and water mixture did not significantly deteriorate, indicating that water effectively protected the pores of zeolite to prevent excessive adsorption of AA. This was attributed to the fact that water was adsorbed by Brønsted acid sites of ZSM-5 more preferentially than AA, thereby avoiding excessive adsorption of AA.
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ChemCatChem
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2025
·
IF 3.9
Juan Meng,Shuhao Chen,Yihui Li,Minnan Liu,Yue Zhou,Long Cheng,Hengfei Qin
This study presents the synthesis of a V 2 O 5 -NiO nanosheets composite catalyst via a straightforward hydrothermal method, aiming to explore the relationship between its microstructural features and its performance in the 5-hydroxymethylfurfural oxidation reaction (HMFOR). The analysis revealed a notable increase in the concentration of oxygen vacancies in the V 2 O 5 -NiO composite compared to pure V 2 O 5 , indicating an enhanced catalytic capacity. The V 2 O 5 -NiO electrocatalyst achieved an impressive 2,5-Furandicarboxylic acid (FDCA) conversion rate of 96.7%, demonstrating excellent electrochemical activity. Moreover, the catalyst exhibited remarkable stability, maintaining high conversion efficiencies for both 5-Hydroxymethylfurfural (HMF) to FDCA over multiple cycles. These results emphasize the critical role of oxygen vacancies and the synergistic interaction between V 2 O 5 and NiO in optimizing catalyst performance. This work provides important insights into the design of robust, efficient electrocatalysts, advancing the sustainable production of FDCA from HMF. Graphical A V 2 O 5 -NiO nanosheet electrocatalyst, synthesized through a hydrothermal process, demonstrates a remarkable 96.7% yield of FDCA in the electrocatalytic oxidation of HMF. This result underscores the significance of oxygen vacancies and the synergistic interaction between V 2 O 5 and NiO in improving the catalyst's performance, making it a promising candidate for sustainable biomass conversion.
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ChemCatChem
·
2021
·Vol. 13
·期 16
·3601-3610
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IF 5.686
Bing Xu,Minghui Tan,Xuemei Wu,Hailun Geng,Shengying Zhao,Jie Yao,Qingxiang Ma,Guohui Yang,Noritatsu Tsubaki,Yisheng Tan
Graphical Catalytic propane aromatization : Post-introducing Cr species to Ga/Z5 catalyst had the maximum dehydrogenated active Cr 3+ species. Propane was effectively converted, and more light alkenes from propane dehydrogenation were converted into BTX on 2Cr/GaZ5 catalyst. Active Cr 3+ species and strong interaction between Ga species and ZSM-5 zeolite on 2Cr/GaZ5 catalyst accelerated the dehydrogenation step in propane aromatization. Accelerating propane dehydrogenation in propane aromatization is vital because it is the first and rate control step. In this study, we introduced Cr to Ga/ZSM-5 by tuning its impregnation sequence and amount, which was expected to accelerate the dehydrogenation step and improve aromatization performance. The impregnation sequence of Cr on catalyst not only affected the interaction between Ga and ZSM-5, but also tuned the amount of dehydrogenation active species Cr 3+ . Due to the plenty of Cr 3+ species and strong interaction between Ga species and ZSM-5, 2Cr/GaZ5 catalyst accelerated the dehydrogenation step and improved the aromatization process. More light hydrocarbons were preferred to be produced and were further converted into BTX on 2Cr/GaZ5 catalyst. Excessive Cr on catalyst caused the formation of Cr 2 O 3 particles with worse dispersion. The aggregated Cr 2 O 3 decreased the strong acidity of catalyst, which could not further promote propane conversion and decreased the aromatization ability of catalyst.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Suwen Wang,Menghui Qi,Shanjun Mao,Kai Liu,Yong Wang
Engineering a phosphate-anchored proton-shuttling interfacial microenvironment on NiCo hydroxides. • Reversible PO 4 3− /HPO 4 2− interconversion accelerates the kinetics of hydrogen transfer process. • Achieving near-quantitative FDCA yield and robust stability in an MEA electrolyzer. • Validating the proton-shuttling strategy for oxidative upgrading of diverse biomass substrates. The rational design of interfacial microenvironments that regulate proton transfer is crucial for overcoming the kinetic bottleneck of proton-coupled electron transfer (PCET) in electrocatalytic biomass oxidation. Herein, we propose a phytic acid (PA)-derived phosphate modification strategy to construct a phosphate-mediated proton-transfer-regulated interface in NiCo(OH) x -PA for efficient 5-hydroxymethylfurfural (HMF) electrooxidation. Unlike conventional static ligand modification and active-site regulation strategies, phosphate groups utilize their Lewis basicity to regulate interfacial proton-transfer kinetics through reversible PO 4 3 ⁻/HPO 4 2 ⁻ interconversion, thereby promoting the Ni 2+ /Ni 3+ redox cycle during HMFOR. Operando spectroscopic characterization and theoretical calculations reveal that phosphate groups serve as dynamic proton relays to facilitate proton-transfer coupling between Ni 2+ -OH activation and HMF dehydrogenation, lowering the energy barrier of key reaction steps and enhancing HMFOR selectivity over the competing OER pathway. Consequently, the optimized NiCo(OH) x -PA catalyst achieves nearly quantitative FDCA Faradaic efficiency and excellent stability over 55 consecutive cycles. This phosphate-mediated proton-transfer-regulated interface provides a new strategy for designing efficient electrocatalytic biomass upgrading systems. Download: Download high-res image (168KB) Download: Download full-size image A phytic acid (PA)-induced surface reconstruction strategy is developed to accelerate proton-coupled electron transfer (PCET) during HMF electrooxidation. Surface-anchored phosphate groups act as proton shuttles, facilitating rapid deprotonation and boosting HMF-to-FDCA conversion with nearly 100% yield and Faradaic efficiency. This work provides a ligand-engineering paradigm for designing high-performance biomass-upgrading electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiaoping Liu,Yunbo Zhai,Zhixiang Xu,Yun Zhu,Yin Zhou,Zhexian Wang,Liming Liu,Fashen Liang,Wanying Ren,Yu Xie,Caiting Li,Min Xu
Natural deep eutectic solvents (NADES) coupled with hydrothermal treatment was innovatively proposed to process waste activated sludge for sustainable production of 5-methylfurfural (5-MF) and enhanced dewaterability. The yield of 5-MF up to 11.54 kg/t volatile solids (VS) with a NADES dosage of 2.0 mL, hydrothermal temperature of 180 °C and holding time of 30 min. The decreased capillary suction time (CST) and bound water content indicated that NADES with hydrothermal treatment substantially improved the dewaterability of sludge. The variations of sludge physicochemical properties and extracellular polymeric substances (EPS) compositions revealed that NADES disrupted the structure of sludge biopolymers. Density functional theory (DFT) calculations indicated that NADES weakened the hydrogen bond strength between EPS components, and thus promoted the solubilization of proteins and polysaccharides. Besides, transition state analysis showed that NADES also lowered the energy barrier of polypeptide hydrolysis and carbohydrates dehydration reactions for the production of 5-MF.
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AMERICAN JOURNAL OF PATHOLOGY
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2025
·Vol. 195
·期 12
·2320-2335
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IF 3.6
Jing Li,Meixue Chen,Lingling Lu,Yinmiao Wang,Wei Wu,Yanhong Feng
Pediatric asthma is a respiratory disease in which M2 macrophages play a critical role. Here, the role and molecular mechanism of lysophosphatidic acid receptor 5 ( LPAR5 ) were investigated in pediatric asthma through in vivo and in vitro experiments. LPAR5 expression was increased in peripheral blood mononuclear cells from children with asthma. In an ovalbumin-induced neonatal asthmatic mouse model, LPAR5 antagonist alleviated airway inflammation by suppressing the release of inflammatory cytokines and inflammatory cell infiltration. Ovalbumin-induced M2 macrophage activation in neonatal mouse lung tissue was suppressed by LPAR5 antagonist, accompanied by decreased YM1 protein (encoded by chitinase 3 like 1) secretion. Differentiated THP-1 cells were stimulated with IL-4 to mimic M2 macrophages in vitro . M2 macrophage activation was reduced by both LPAR5 antagonist or LPAR5 knockdown. Furthermore, KLF transcription factor 5 ( KLF5 ) was significantly up-regulated and positively correlated with LPAR5 expression in peripheral blood mononuclear cells from children with asthma. KLF5 bound to the promoter of LPAR5 and transcriptionally promoted LPAR5 expression. LPAR5 overexpression increased M2 macrophage activation in KLF5-depleted THP-1 cells. The underlying mechanism of LPAR5 was investigated by phosphorylomics analysis, which identified mitogen-activated protein kinase kinase kinase 7 as a possible downstream effector. The results showed that LPAR5 antagonist attenuated airway inflammation in neonatal mice by decreasing M2 macrophage activation. KLF5 positively regulates the expression of LPAR5, which further increased the phosphorylation of mitogen-activated protein kinase kinase kinase 7 protein in macrophages. This article highlights that LPAR5 might serve as a potential target in pediatric asthma.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Yinglu Chen,Yitao Yan,Jie Chen,Ben Zheng,Youwei Jiang,Zhengzhong Kang,Jun Wu
Given the prevalence of the malignant weed Chinese Sprangletop (Leptochloa chinensis (L.) Nees) in rice fields, the development of novel herbicides against this weed has aroused wide interest. Here, we report a novel diphenyl ether-pyrimidine hybrid, DEP-5, serving as a systematic pre/postemergence herbicide candidate for broad-spectrum weed control in rice fields, specifically for L. chinensis. Notably, DEP-5 exhibits over 80% herbicidal activity against the resistant biotypes even at 37.5 g a.i./ha under greenhouse conditions and has complete control of L. chinensis at 150 g a.i./ha in the rice fields. We uncover that DEP-5 acts as a noncompetitive inhibitor of acetohydroxyacid synthase (AHAS) with an inhibition constant (Ki) of 39.4 μM. We propose that DEP-5 binds to AHAS in two hydrophobic-driven binding modes that differ from commercial AHAS inhibitors. Overall, these findings demonstrate that DEP-5 has great potential to be developed into a herbicide for L. chinensis control and inspire fresh concepts for novel AHAS-inhibiting herbicide design.
研究领域:
植物学
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农业科学
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分子生物学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Heng Ban,Youwei Cheng,Lijun Wang,Xi Li
2,5-Furandicarboxylic acid (FDCA) derived from biomass is a versatile platform chemical for producing various degradable polymers, especially polyethylene 2,5-furandicarboxylate (PEF). To reduce the high cost of feedstock, fructose instead of expensive 5-hydroxymethylfurfural (HMF) was used as the feedstock for producing FDCA in the acetic acid (HOAc) solvent by a one-pot, two-step method. Fructose was first catalytically converted into HMF and 5-acetoxymethylfurfural (AMF) in HOAc over the Amberlyst-15 catalyst. After the separation of only Amberlyst-15, the in situ-formed HMF and AMF were further catalytically oxidized to FDCA by air (oxygen) over homogeneous Co/Mn/Br catalysts following the free-radical chain reaction mechanism. HOAc was not only used as the solvent for the dehydration and following oxidation process but also served as the effective co-catalyst for the dehydration of fructose. The effects of catalyst species, dosage, and reaction temperature on the dehydration process and oxidation temperature on FDCA yield and purity were evaluated systematically. Under the optimized reaction conditions, a total yield of HMF and AMF of 50% and a final FDCA yield of 35% were achieved. Combined with experimental results and theoretical calculation, the reaction mechanism for fructose dehydration side reactions and the HMF and AMF oxidation reactions was proposed correspondingly. The proposed two-step, one-pot method using fructose as the starting material is a promising route for the commercial production of FDCA with the simple operation and viable yield.
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Molecular Catalysis
·
2026
·
IF 4.3
Shukang Ti,Dongmei Yue
Pd/DUT-5 is an efficient catalyst for NBR hydrogenation to HNBR. • High hydrogenation activity was achieved under mild conditions. • Metal-support interactions stabilize electron-enriched Pd δ+ species. • Pd δ+ species enhance catalytic activity and chemoselectivity. • DFT reveals low-barrier heterolytic H 2 activation at Pd δ+ –μ 2 O - sites. Hydrogenated nitrile butadiene rubber (HNBR), produced via the selective hydrogenation of nitrile butadiene rubber (NBR), has attracted considerable interest because of its excellent overall performance. However, the development of efficient and selective catalytic systems for NBR hydrogenation under mild conditions remains challenging, particularly when both activity and cost-effectiveness are required. Herein, Pd nanoparticles were immobilized on the Al-based metal-organic framework DUT-5, and the influences of Pd precursor salts and pretreatment conditions on catalytic hydrogenation performance were systematically investigated. The results show that using Pd(OAc) 2 as the precursor in combination with relatively low reduction temperatures promotes the formation and stabilization of electron-enriched Pd δ+ species through metal-support interactions, leading to excellent low-temperature activity and good reusability, with the hydrogenation degree remaining 94.5% after three cycles. Density functional theory calculations using C 2 H 4 as a model substrate further reveal that Pd δ+ sites cooperatively interact with μ 2 O - moieties to facilitate H 2 activation and subsequent hydrogen transfer through a heterolytic cleavage pathway with reduced energy barriers. These results provide a mechanistic basis for the efficient hydrogenation of NBR under mild conditions. Overall, this work demonstrates an effective and economical strategy for HNBR production and offers new insights into the design of highly active and chemoselective catalysts for NBR hydrogenation. Download: Download high-res image (205KB) Download: Download full-size image
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