CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lingxi Bai,Haonan Li,Xingxiang Wang,Xin Pu,Zhipeng Lin,Shuzhen Zhou,Jiangbing Li,Xiaogang Wang,Jie Li,Lingtao Kong,Lanli Bai,Jichang Liu
Biomass valorization plays a vital role in ecological conservation and the advancement of a circular economy, while posing significant scientific challenges. This work successfully constructed a novel tandem catalytic system (ZnZrOx-ZSM-5) for the efficient production of sustainable monocyclic aromatics (SMAs) via the ex-situ catalytic pyrolysis of cotton stalk. Compared to the sole ZSM-5, the tandem catalyst significantly enhanced the absolute yield of SMAs from 8.2 % to 26.8 %. Combined various structural characterization and carefully catalytic experiments, it was revealed that pyrolysis volatiles derived from cotton stalk first encounter the ZnZrOx bed-rich in oxygen vacancies and basic sites, where compounds such as AAAKs (alcohols, aldehydes, acetic acid, and ketone) and bulky alkoxy-phenols are preferentially pre-cracked into alkanes/alkenes and light phenols, respectively. Subsequently, within the ZSM-5 bed, these pre-cracked intermediates enhance the formation of SMAs by a series of reactions-including Diels-Alder condensation, dehydroxylation, and aromatization with hydrocarbon pool species. Simultaneously, GC‑MS analysis confirmed that the introduction of ZnZrOx effectively suppresses the formation of bulky polycyclic molecules (e.g., naphthalene, phenanthrene), thereby alleviating catalyst pore blockage and deactivation.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Jirong Long,Yuxuan Mao,Yiwei Long,Guozhang Chang,Lungang Chen,Wenguang Zhou,Jinxing Long,Yong Liu
Hydrodeoxygenation of lignin-derived phenols into high-value cycloalkanes under mild conditions is challenging. Herein, we report a Ru NPs @HZSM-5 catalyst with a unique metal-support interactions that achieves 100 % guaiacol conversion and 99.7 % cyclohexane selectivity at 160 °C and 1 MPa H 2 . Comparative studies with single-atom and aggregated Ru catalysts reveal that well-dispersed Ru nanoparticles coupled with acid sites offer superior activity and selectivity. Kinetic analysis and in situ DRIFTS demonstrate a sequential mechanism involving rapid hydrogenation of the aromatic ring followed by rate-limiting deoxygenation steps. Characterizations and CO-DRIFTS confirm particle sizes, optimal metal-support interactions, and enhanced acidity in Ru NPs @HZSM-5. Theoretical calculations further reveal favorable electronic states and lower energy barriers for deoxygenation on Ru NPs @HZSM-5. The catalyst also shows broad substrate compatibility, efficiently converting various lignin-derived phenolics. This work provides valuable insights into the critical synergy between metal nanoparticles and acidic supports for efficient lignin upgrading.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Huan Wen,Xizi Wu,Zelong Sun,Zhangyue Zheng,Junxin Chen,Jia Wu,Shibin Yin
The 5-hydroxymethylfurfural electrooxidation reaction (HMFOR) stands out due to the value-added production and mild conditions. However, its catalytic efficiency is hampered by sluggish kinetics. Herein, with a focus on optimizing the adsorption and activation of reaction molecules, a Co 5.47 N-W 5 N 4 heterostructure catalyst is constructed for efficient HMFOR. The heterogeneous interface formed between Co 5.47 N and W 5 N 4 synergistically enhances the adsorption and activation of substrate molecules through electronic structure modulation and dual-site hydrogen bonding interactions. Meanwhile, the interfacial electron transfer from Co 5.47 N to W 5 N 4 facilitates the formation of high-valent cobalt species (Co 3+ /Co 4+ ), which is critical for activating formyl and hydroxymethyl groups. Furthermore, the hierarchical nanoparticle-nanosheet architecture provides abundant active sites while promoting efficient mass transport. These combined effects render Co 5.47 N-W 5 N 4 with enhanced HMFOR performance, along with a 5.80-fold increase in the rate constant for the rate-determining step. This work puts forward an approach for developing efficient HMFOR catalysts by promoting the adsorption and activation of reaction molecules.
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PubMed
高影响因子
Synthetic and Systems Biotechnology
·
2025
·
IF 4.4
Yanghao Liu,Changgeng Li,Yu Miao,Zhichao Chen,Tangen Shi,Ling Ma,Siyu Zhao,Zichen Yu,Lanxiao Li,Qingyang Xu
5-Aminolevulinic acid (5-ALA) is an important non-proteinogenic amino acid with wide applications in agriculture and medicine. To achieve high-level microbial production, this study established a dual-pathway reconstruction strategy in Escherichia coli by integrating the endogenous C5 pathway with an inducible exogenous C4 pathway. Multi-copy overexpression of gltX , hemA , and hemL , combined with enhanced glutamate supply and the introduction of a non-oxidative glycolysis pathway, effectively increased the C5 pathway flux and carbon efficiency, while product toxicity was significantly alleviated by strengthening efflux mechanisms and oxidative stress tolerance. A quorum sensing–based regulatory system was employed to dynamically regulate hemB expression, thereby balancing cell growth and 5-ALA biosynthesis, and a controlled glycine feeding strategy specifically activated the C4 pathway during the later fermentation stage, forming a stage-specific dynamic activation mechanism. Promoter regulation of sucC/sucD expression and enhanced endogenous PLP biosynthesis further stabilized the C4 flux. Fed-batch fermentation in a 5 L bioreactor resulted in a final 5-ALA titer of 37.34 g/L, demonstrating the industrial potential of this systems metabolic engineering strategy combining dual pathways and stage-specific activation control.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shichao Peng,Hua Li,Wenjuan Liu,Junyi Yu,Zhaochao Xu,Mao Ye,Zhongmin Liu
Mass transfer of guest molecules is crucial for zeolite catalysis. Compared to intracrystalline diffusion, the surface barriers in zeolite catalysis have been less understood. Taking furfuryl alcohol oligomerization catalyzed by ZSM-5 zeolites as model reaction, here we present a single-crystal level study and gain insight into the surface barriers induced spatiotemporal evolution of oligomer products using structured illumination microscopy (SIM). It is shown that, as a result of the enhanced accessibility to zeolite crystals, promoting the surface permeability leads to the increase in catalytic reaction rate that is characterized as the generation rate of oligomer products.
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Changfei Zou,Li Yang,Kaili Luo,Lei Liu,Xiyuan Tao,Lingguang Yi,Xianhu Liu,Zhigao Luo,Xianyou Wang
All-solid-state lithium metal batteries (ASSLMBs) with argyrodite-type Li6PS5Cl solid electrolyte (SE) show potential to replace current commercially available lithium-ion batteries by virtue of their potentially high energy density and safety. However, the interface incompatibility between sulfide solid electrolyte and lithium metal leads to an increase in interfacial resistance and the rapid growth of lithium dendrites, which greatly impede its commercial application. To alleviate the above problems, here a cell construction model has been put forward, in which composite polymer electrolytes (CPEs) with high ionic conductivity and good interface compatibility against lithium metal are employed as the interphase between Li6PS5Cl solid electrolyte and lithium metal. CPEs can prevent direct contact between lithium anode and Li6PS5Cl, and a soft CPE layer can solve the problem of high interfacial resistance caused by bad contact between the Li6PS5Cl solid electrolyte and the lithium metal anode. As a result, the symmetric cells Li/CPEs/Li6PS5Cl/CPEs/Li show stable polarization voltage over 140 h at a current density of 0.2 mA at 60 °C. Compared with the rapidly decaying capacity of the LiFePO4/Li6PS5Cl/Li cell, the initial discharge capacity of LiFePO4/Li6PS5Cl/CPEs/Li is 93.74 mAh/g, and after 15 cycles at 0.5 C, the capacity retention rate is still 75.1%. Therefore, the successful design of this cell structure based on the interface modification of Li6PS5Cl solid electrolyte provides good prospects for the commercial application of ASSLMBs.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2013
·Vol. 38
·期 2
·845-851
·
IF 2.966
Li-Li Tan,Yumo Zhang,Bao Li,Kai Wang,Sean Xiao-An Zhang,Yanchun Tao,Ying-Wei Yang
Highly selective binding of “solvent” molecules by 1,4-dimethoxypillar[5]arene (DMP[5]A) and their host–guest complexation in solution and the solid state have been investigated by multiple methods. Enthalpy changes and the size-fit effect play an important role in the high selectivity.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·Vol. 29
·期 60
·e202301827
·
IF 4.3
Mengyan Zeng,Xin Chen,Jie Zhang
Hierarchical chiral structures have broad applications in optical devices, asymmetric catalysis, and biological systems. The delicate balance of various interactions are key to the self-assembly of chiral structures. Herein, a ternary co-assembly consisting of cationic pillar[5]arenes (P5As), anionic β- glucopyranoside ( β GlcD/ β GlcL), and Anderson-type polyoxometalates (POMs) were constructed. Through adjusting the stoichiometry of β GlcD, the assemblies were effectively controlled to form hierarchical nano-leaf assemblies with twisted nanoribbons in a homochiral direction. The co-assemblies exhibit strong Cotton effects, and successfully induced the chirality of Anderson-type POMs. More interestingly, by changing the central metal in Anderson-type POMs (XMo 6 O 24 3− (X=Cr, Al, and Ga)), even though the three clusters have the same numbers of charge and size, the hierarchical chirality of the related assemblies varied in the morphology of the assemblies and the Cotton effect in the CD spectra. Results in theoretical calculations and ITC titration indicates that the tiny difference in long-range electrostatic interaction would result in the anion recognition of POMs, modulated by β GlcD through host–guest inclusion and hydrogen bonding in the assembly process. Graphical β -Glucopyranoside, as a modulator, successfully induced the chirality of Anderson-type polyoxometalates and modulated the ternary co-assembly to form hierarchically chiral leaves. By substituting highly similar polyoxometalates, the accurate balance between short- and long-range interactions is demonstrated to be the key to the formation of chiral hierarchical microstructures.
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高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 31
·e202300799
·
IF 2.1
Lin-Jie He,Yao-Feng Wang,Peng-Xin Guan,Qing-Shan Niu,Hong-Ying Liu,Bao-Hua Xu
The vapor-phase nitrilation of dimethyl adipate (DMA) with ammonia (NH 3 ) is an environmentally benign route leading to adiponitrile (ADN) with great application value. In this study, the performance of HZSM-5 zeolites, widely used in industry as the solid acid catalysts, was investigated. It exhibits a strong correlation between the SiO 2 /Al 2 O 3 ratio (SAR) in HZSM-5 zeolites and the reactivity (both activity and selectivity). The influence of Al density closely related to the value of SAR on the reactivity of HZSM-5 was thus elucidated by mechanistic experiments. As a result, the introduction of Al element to the framework is beneficial to the activation of ester functionality, thus improving the activity, especially at a high liquid hourly space velocity (LHSV). However, a high Al density will lead to poor selectivity and deactivation due to too strong adsorption of esters and intermediates (e. g., amides). Herein, the balanced adsorption/desorption capability was reached on HZSM-5 with SAR as 631 (i. e., HZSM-5-631), which provides the best selectivity to nitriles (S ADN+MCP , 92.5 %) at a high single-pass conversion of DMA (C DMA , 98.0 %). Graphical The nitrilation of DMA over HZSM-5 with different SiO 2 /Al 2 O 3 was investigated, wherein HZSM-5 with SiO 2 /Al 2 O 3 of 631 exhibited excellent reactivity due to the balance of ester activation and amide intermediate desorption.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yu Tian,Huina Liu,Jianan Li,Yuanyuan Ding,Manman Zhu,Chenguang Liu
A multiscale engineering strategy integrates THEDES with thermosensitive hydrogels. • THEDES enhances 5-ASA solubility, permeability, and anti-inflammatory efficacy. • THEDES-Gel enables prolonged colonic retention and controlled release. • THEDES-Gel provides a versatile platform for insoluble drugs for UC treatment. Overcoming the low aqueous solubility, poor mucosal permeability, and imprecise delivery of drugs remains a critical challenge in pharmaceutical engineering. Herein, we designed a novel therapeutic deep eutectic solvent (THEDES) using 5-aminosalicylic acid (5-ASA) and L-arginine (Arg) at a molar ratio of 1: 1.4, which functioned as both a solubilizer and osmotic enhancer of 5-ASA. THEDES showed satisfactory viscosity (61.7 ± 1.3 Pa·s), pH (8.9), zeta potential (−12.0 ± 1.4 mV), and anti-inflammatory activity when using in colonic microenvironment. To address the subsequent challenges of rapid clearance and leakage of THEDES at the colon lesion site, THEDES was loaded into a poloxamer 407 hydrogel with methylcellulose as the adhesive to construct an in-situ gelling enema system (THEDES-Gel). Notably, the engineered THEDES-Gel significantly prolonged colonic retention compared to THEDES alone, while achieving a high cumulative release rate of 5-ASA (97.0 ± 0.8% at 6 h) under the effect of “Push-Pull-Permeate”. Furthermore, THEDES-Gel was demonstrated to have a significant alleviating effect during the treatment of UC in mice by reducing inflammation and maintaining the normal structure of colonic tissue. THEDES-Gel demonstrates a rational materials design strategy that couples molecular-scale solvent engineering of drugs with macroscopic drug delivery system fabrication for the efficient utilization of insoluble drugs.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Peng Shan,Hong Wang,Zhihang Xu,Yilin Wang,Chenglong Fu,Jinwen Hu,Yehan Tao,Xiaodong Xia,Jian Du,Haisong Wang
An adsorption-triggered mechanism was proposed for on-demand release. • Acidic sites on ZSM-5/ZIF-8 possess stronger adsorption energy for biogenic amines than CA. • The mechanical and gas barrier of film were improved after introducing ZSM-5/ZIF-8. • The developed packaging effectively prolonged fish preservation at 4 °C. Active packaging with on-demand release capability has attracted increasing interest in food preservation; however, the delayed response of active agents often compromises protection during the early stage of spoilage. In this work, an adsorption-triggered release strategy was proposed by incorporating cinnamaldehyde (CA)-loaded ZSM-5/ZIF-8 nanoparticles (CA@ZSM-5/ZIF-8) into a sodium alginate (SA) matrix. Owing to the strong affinity of biogenic amines toward the adsorption sites of ZSM-5/ZIF-8, low concentrations of histamine could competitively displace the preloaded CA, thereby enabling an early and responsive release behavior. In the absence of histamine, the cumulative release of CA from the composite film remained below 10% within 12 h, whereas it increased to approximately 60% in the presence of 5.0 mM histamine. Meanwhile, the optimized film exhibited improved tensile strength (54.6 MPa), water vapor barrier performance (0.86 × 10 −10 g·m·m −2 ·s −1 ·atm −1 ), UV-shielding capability, and water resistance. The film also showed pronounced antioxidant activity (91.4%), sustained antibacterial effects against E. coli and S. aureus , and favorable biodegradability. When applied to fish preservation, the optimized film effectively extended the refrigerated shelf life to 6 days at 4 °C. This study provides a novel paradigm for on-demand release in intelligent food packaging.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 32
·16970-16984
·
IF 3.9
Li Lingfeng,Xiong Yongzhi,Huang Yuxin,Zhang Yiling,Li Chenge,Liu Qi,Zhou Junfang,Wang Yihan,Chen Changzhou,Wang Kui,Jiang Jianchun
In this study, we present a straightforward synthesis
strategy
to prepare transition metal sulfide electrocatalysts supported on
sulfonated carbon nanotube-chitosan-derived carbon aerogel. Highly
dispersed Ni 3 S 2 @CNT, Cu 7 S 4 @CNT, and Co 4 S 3 @CNT were successfully fabricated
and applied for 5-hydroxymethylfurfural (HMF) electrooxidation to
2,5-furandicarboxylic acid (FDCA). Among them, Co 4 S 3 @CNT exhibited remarkable electrocatalytic activity, delivering
a current density of 100 mA cm –2 at a low potential
of 1.367 V (vs RHE) while attaining 99.82% HMF conversion, 99.97%
FDCA selectivity and a Faradaic efficiency of 83.75%. Electrochemical
measurements revealed that Co 4 S 3 @CNT possesses
an electrochemical active surface area (ECSA) of 0.781 μF cm –2 , which is higher than those of Ni 3 S 2 @CNT and Cu 7 S 4 @CNT, implying an increased
population of active sites and enhanced catalytic activity. In-situ
Raman spectroscopy reveals that Co 4 S 3 @CNT undergoes
a progressive reconstruction from Co(OH) 2 to CoOOH under
anodic conditions, with CoOOH formation being significantly delayed
in the presence of HMF, confirming its role as the active phase. Density
functional theory (DFT) calculations further indicate that the excellent
performance of Co 4 S 3 @CNT originates from the
lowest energy barrier (1.84 eV) for the rate-determining catalyst
activation dehydrogenation step, coupled with its pronounced charge-polarization
capability that facilitates HMF preactivation. This work gives a promising
design approach for developing efficient nonprecious metal electrochemical
catalysts toward biomass valorization.
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高影响因子
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