CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2026
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IF 3.5
Cai He,Bingfeng Guo,Tong Li,Xiaoxia Jia,Yong Wang,Zhiyun Xiao
A rigid–flexible Zn-DMOF was developed for selective C 2 H 2 /CO 2 separation. • Activation-induced pore contraction enabled dynamic recognition of C 2 H 2 . • Zn-chdc-DABCO retained high C 2 H 2 uptake but greatly improved C 2 H 2 /CO 2 selectivity. • Efficient breakthrough separation was maintained under varying flow rates and humidity. Separating C 2 H 2 from CO 2 is challenging because of their similar sizes and physicochemical properties. Adsorption-based separation using metal–organic frameworks (MOFs) offer a promising alternative. Here, a rigid–flexible framework strategy is used to introduce guest-discriminating dynamic recognition into a 1,4-diazabicyclo[2.2.2]octane (DABCO)-based MOF (DMOF) platform by replacing rigid 1,4-benzenedicarboxylate with flexible trans-1,4-cyclohexanedicarboxylate, affording Zn-trans-1,4-cyclohexanedicarboxylic acid (chdc)-DABCO. Activation induces pore contraction and generates a confined environment that selectively strengthens C 2 H 2 binding while leaving CO 2 largely unaffected. As a result, Zn-chdc-DABCO preserves a C 2 H 2 uptake comparable to that of Zn-DMOF at 298 K and 100 kPa, yet displays markedly enhanced affinity toward C 2 H 2 , a distinct gate-opening response to C 2 H 2 , and little framework response toward CO 2 . The zero-coverage isosteric heat of adsorption reaches 43.9 kJ·mol –1 for C 2 H 2 , substantially higher than that for CO 2 (29.3 kJ·mol –1 ), and the equimolar C 2 H 2 /CO 2 ideal adsorbed solution theory selectivity reaches 8.2, more than four times that of Zn-DMOF. Dynamic breakthrough experiments further confirm efficient separation under mixed-gas, variable-flow, and humid conditions. This work shows that rigid–flexible cooperative design offers an effective route to overcoming the capacity/selectivity trade-off in difficult gas separations. A rigid–flexible Zn-DMOF was engineered to enable activation-induced pore contraction and guest-discriminating dynamic recognition, thereby achieving enhanced selective C 2 H 2 /CO 2 separation with efficient C 2 H 2 recovery. Download: Download high-res image (204KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Ziyang Xu,Huiduo Li,Zicheng Yang,Yi Feng,Jianfeng Yao
Air-induced self-reduction creates abundant coupled Mo 5+ –oxygen vacancy pairs. • Poisoning experiments identify Lewis acidic Mo ions as the true active centers. • Lamellar-stacked architecture exposes high-density active sites for CO 2 conversion. • The catalyst displays excellent cycling stability and broad substrate adaptability. CO 2 cycloaddition provides a sustainable and atom-economical route for CO 2 utilization, yet the development of high-performance molybdenum-based catalysts is hampered by poorly controllable defect modulation and ambiguous active-site origins. Herein, we report a facile air calcination strategy to fabricate lamellar-stacked defective molybdenum oxide (Mo-MOF-500/2h) from a rod-shaped Mo-MOF precursor. Air-induced pyrolysis enables the in-situ formation of abundant Mo 5+ species along with oxygen vacancies, fundamentally different from the isolated inert oxygen vacancies in conventional MoO 3 . Selective chemical poisoning experiments and kinetic analysis resolve the long-standing controversy regarding active sites in Mo-based cycloaddition catalysis, verifying that Lewis acidic Mo 5+ /Mo 6+ centers rather than surface hydroxyl groups dominate epoxide activation, while adjacent oxygen vacancies modulate paired Mo 5+ centers to lower the apparent activation barrier. As a result, Mo-MOF-500/2h achieves a high carbonate yield of 96% for CO 2 cycloaddition with epichlorohydrin within 6 h at 80 °C under atmospheric CO 2 pressure, accompanied by good substrate adaptability and excellent long-term cycling durability. This work clarifies the morphology–defect–activity correlation of molybdenum oxides and provides feasible guidance for the design of high-efficiency CO 2 fixation catalysts. Download: Download high-res image (221KB) Download: Download full-size image
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ACS Sustainable Chemistry & Engineering
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2026
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IF 7.6
Wang Hongsheng,Zeng Yue,Lyu Shuai,Xiao Ping,Hadizadeh Mohammad Hassan,Wang Shan,Zhu Junjiang
Cu−Co bimetallic catalysts have demonstrated considerable potential for CO 2 hydrogenation to C 2 + alcohols. However, their practical application remains constrained by excessive CH 4 formation arising from the uncontrolled reduction of Co species under reaction conditions. Herein, we report a semi-encapsulated catalyst architecture constructed through a lattice-mismatching strategy. The lattice mismatch between hexagonal CoO (h-CoO) and ZnO is only 0.18%, whereas that between Cu 2 O and ZnO reaches 31.4%. When ZnO serves as the seed crystal, Cu 2 O preferentially nucleates and grows into nanoparticles on the ZnO surface, while h-CoO undergoes epitaxial growth on the exposed ZnO regions, forming a semi-encapsulated configuration in which Cu 2 O nanoparticles are partially confined by an h-CoO overlayer. The strong lattice matching between h-CoO and ZnO stabilizes Co species in an oxidized state under reaction conditions, thereby suppressing the formation of metallic Co and CH 4 production. Meanwhile, the confinement effect imposed by the h-CoO overlayer effectively restricts Cu migration, preserving the Cu−Co interfacial sites that are critical for C−C coupling. As a result, the optimized catalyst achieves a C 2 + alcohol selectivity of 63.7% at 300 ° C, with an ethanol selectivity of 30.0%, and exhibits no noticeable deactivation over 200 h of continuous operation. This work demonstrates that lattice-matching-directed interfacial engineering represents an effective strategy for simultaneously regulating active-phase stability and metal dispersion, offering new insights into the rational design of catalysts for selective CO 2 hydrogenation to C 2 + alcohols.
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高影响因子
ACS Nano
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2026
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IF 17.3
Shiqun Wu,Chenggui Zhong,Lijie Wang,Ruijie Yang,Ziwei Ye,Chengxuan He,Mingyang Li,Jinlong Zhang
Selective photocatalytic reduction of CO2 to CH3COOH is highly desirable but hindered by poor intermediate stabilization and sluggish C–C coupling. Here we report a coordination-environment engineering strategy to construct asymmetric Co active sites and induce intrinsic spin polarization by nitrogen incorporation into Co3O4. Nitrogen substitution and oxygen vacancy formation generate Co sites with distinct coordination and charge distributions, stabilizing *CO intermediates and lowering the C–C coupling barrier. Concurrently, spin polarization enhances charge carrier separation, further intensified by an external magnetic field. In situ spectroscopy and theoretical calculations confirm the synergistic role of asymmetry and spin effects in facilitating intermediate formation and CH3COOH production. The optimized N–Co3O4–X catalyst achieves a CH3COOH yield of 41.4 μmol g–1 h–1 with 95% electron selectivity under external magnetic field. This work presents a dual-modulation strategy for efficient CO2-to-C2 conversion.
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PubMed
高影响因子
ACS Applied Nano Materials
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2026
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IF 5.8
Luoning Li,Xiaozhuo Zhao,Guocan Jiang,Jinlin Yin,Sheng Li,Zhengquan Li,Jin Wang
Heavy-metal-free photocatalysts for solar-driven CO2 reduction represent a sustainable pathway toward carbon-neutral fuel production. Ternary chalcogenide AgInS2 (AIS) quantum dots (QDs), nanoscale semiconductors (typically 2–5 nm) whose optoelectronic properties are intrinsically governed by quantum confinement and high surface-to-volume ratios, offer an environmentally benign alternative but suffer from insufficient reduction potential and rapid charge recombination. In this work, we demonstrate that Ga3+ doping into AIS (AIGS) QDs simultaneously engineers band edges and suppresses defect-mediated charge recombination. Systematic compositional tuning of AIGS QDs yields optimized photocatalytic CO2 reduction performance, achieving CH4 and CO production rates of 16.7 μmol g–1 h–1─a 6.2-fold improvement over pristine AIS QDs. Combined spectroscopic, electrochemical, and density functional theory investigations establish that Ga3+ doping upshifts the conduction band minimum to enhance thermodynamic driving force while reducing defect states that serve as recombination centers. Transient spectroscopy confirms prolonged charge-carrier lifetimes in AIGS QDs, directly correlating with improved photocatalytic performance. This integrated band engineering and defect passivation strategy provides an efficient way for designing high-performance, heavy-metal-free QD photocatalysts for artificial photosynthesis.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Guowei Chen,Yang He,Shen Xiang,Yiping Zhao,Li Chen
Oxygenation membranes for extracorporeal membrane oxygenation systems require ultrathin, defect-free selective layers that simultaneously deliver high gas permeability, selectivity, and operational stability. Herein, we report a Janus composite membrane featuring a dense polydimethylsiloxane (PDMS) selective layer integrated with a hydrogen-bonded organic framework (HOF-TGU-307), designed to overcome filler aggregation and transport limitations commonly encountered in ultrathin mixed-matrix membranes. A Marangoni convection-driven assembly strategy induces strong in-plane flow at the gas–liquid-solid interface, enabling uniform dispersion and horizontal embedding of HOF crystallites within the PDMS matrix. Theoretical analysis and molecular dynamics simulations confirm that Marangoni flow suppresses capillary-driven aggregation, while a stable PDMS-HOF interfacial network forms polar gas-transport pathways and promotes interfacial CO 2 enrichment. As a result, the optimized M3-HOF membrane exhibits a high single-gas CO 2 permeance of 1883 GPU and an ideal CO 2 /O 2 selectivity of 5.2, measured at 0.1 MPa and 25 °C, together with an oxygen transfer rate of 219.8 mL·min −1 ·m −2 . The Janus architecture further provides excellent interfacial stability, effectively preventing liquid penetration (LEP > 0.6 MPa). Auxiliary evaluations demonstrate reduced protein adsorption and favorable blood-contacting compatibility, supporting its potential for membrane oxygenators. This computation-guided, Marangoni-driven fabrication strategy offers a scalable route for constructing high-performance oxygenation membrane with controlled ultrathin selective layers.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Yuanwen Shi,Zhenyu Zhao,Hong Li,Xin Gao
Hot spots (δT = 13–40 °C) on adsorbents during MW heating were quantified. • Localized hot spots accelerated the desorption rate by 18%. • Influences of microwave power and N 2 rates on desorption efficiency were studied. • Cyclic regeneration efficiency was improved by 49% using microwave technology. Temperature swing adsorption (TSA) for CO 2 capture generally suffers from slow thermal response and high energy demand during adsorbent regeneration. Microwave swing adsorption (MSA) has emerged as a promising alternative to enable fast regeneration of CO 2 adsorbents. However, the mechanism of microwave-enhanced desorption remains unclear due to the difficulty in determining the actual surface temperature of adsorbents under microwave irradiation. This challenge is overcome in this study by coating a temperature-sensitive fluorescence thermometer onto the adsorbent particles, confirming the existence of a temperature difference (δT) between the adsorbent surface and the bulk bed measured by a fiber-optic sensor. Subsequently, a convective heat transfer model coupled with an electromagnetic heating equation was established to quantitatively predict the influence of purge flow rate and microwave power on δT. The model predictions agree well with the results of systematic experiments with an error < 20%, revealing that MSA can achieve a desorption efficiency at a bulk temperature of 88 °C comparable to that of conventional TSA at 100 °C, therefore reducing the specific regeneration energy consumption by 55% (to 1.91 MJ/kg CO 2 ) and nearly doubling the cyclic processing efficiency. The quantification of hotspot effect drives rational regulation of microwave enhanced CO 2 desorption, thereby advancing the development of energy-efficient carbon capture technologies.
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高影响因子
Nanoscale
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2026
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IF 5.2
Linlong Hu,Chentao Wang,Huibin Wang,Hua Pan,Mi Yan,Ke Wang,Pengfei Xie
CO2 reduction to light olefins is an important pathway toward carbon neutrality, but it is hindered by low thermodynamic conversion and the inherent trade-off between activity and selectivity. To address this challenge, a bifunctional catalyst consisting of Cu single atoms anchored on ZrO2 and SAPO-34 (Cu1/ZrO2-SAPO-34) was developed. This catalyst achieves 84.3% light olefin selectivity and 15.0% CO2 conversion, with stable performance maintained over 100 hours. In this catalyst, Cu single atoms, ZrO2, and SAPO-34 exhibit clear division of labor and synergy, responsible for CO2 activation, active site stabilization, and olefin selectivity control, respectively. Mechanistic investigations using in situ DRIFTS and DFT calculations demonstrate that the interaction between Cu single atoms and ZrO2 facilitates the further hydrogenation of formate intermediates to methoxy species, while reducing the energy barrier for methoxy hydrogenation to methanol, thus ensuring high light olefin selectivity in subsequent conversion over SAPO-34. This work provides new insights for CO2 conversion and the design and application of single-atom catalysts in tandem catalytic reactions.
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PubMed
高影响因子
AICHE JOURNAL
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2026
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IF 4.4
Ziheng Li,Wenji Zheng,Fengting Yao,Zhixu Yun,Yan Dai,Xuehua Ruan,Miao Yu,Tiantian Li,Xiaobin Jiang,Xuemei Wu,Gaohong He
Constructing vertically aligned, penetrating metal–organic framework (MOFs) gas transfer pathways within mixed matrix membranes (MMMs) is an effective strategy for optimizing gas transport under low filler loading (≤25 wt.%). Herein, we developed a novel “stack-polymerize-section” process to construct vertically aligned ZIF-8 pathways in MMMs by tailoring the density and channel size of PAN@ZIF-8 NFM for optimizing CO 2 ultrafast and in-parallel transport. The designed XLPEO/PAN@ZIF-8 MMM exhibits excellent performance far exceeding the 2019 McKeown upper bound, with CO 2 permeability and CO 2 /N 2 selectivity of 369.2 Barrer and 90.0, respectively. Meanwhile, a novel parallel computational model that synergistically integrates the Maxwell model with resistance-based (RB) model methodology was proposed to introduce the interfacial resistance coefficient derived from polymer–MOFs interface heterogeneous concentration gradients. This work demonstrates the potential of vertically aligned MOFs channels for high-performance gas separation, providing a scalable and controllable fabrication pathway for maximizing the efficiency of MOFs in membrane technology.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2026
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IF 3.6
Lang Yu,Yongheng Cui,Zhiliang Lu,Yingjie Zhou,Feng Yan
Utilizing carbon dioxide (CO 2 ) as a renewable C1 building block to produce value-added chemicals represents a key strategy for developing greener and more sustainable chemical processes. Herein, a series of ionic liquids (ILs) with excellent CO 2 activation capabilities was designed and combined with copper(I) chloride to form a synergistic catalytic system. This system efficiently promoted the carboxylative cyclization of propargylic alcohols with CO 2 under mild conditions, such as at room temperature and atmospheric pressure. Among the explored ILs, tetramethyl guanidinium 2,4-dihydroxybenzoate ([TMGH] 3 [2,4-DHBA]) was the most effective catalyst, achieving a conversion of 68.9% for the model substrate 2-methyl-3-butyn-2-ol within 12 h. The superior performance of [TMGH] 3 [2,4-DHBA] is attributed to the presence of multiple CO 2 -philic sites on its anionic scaffold, which significantly enhances the cooperative activation of CO 2 . Furthermore, theoretical simulations revealed that the structural features of the anion play a decisive role in CO 2 adsorption and activation, exhibiting a positive correlation with the overall catalytic activity. This work systematically elucidates, from both experimental and theoretical perspectives, the catalytic mechanism of ILs with different cation–anion combinations in CO 2 transformation reactions, providing critical insights for the rational design of highly efficient and mild catalytic systems for CO 2 utilization. Graphical A synergistic catalytic system combining ionic liquids (ILs) with copper(I) chloride efficiently converts CO 2 into valuable chemicals under mild conditions. The most effective IL, featuring a multi-site CO 2 -philic anion, achieves high conversion by enhancing cooperative CO 2 activation, as validated by experimental and theoretical insights.
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PubMed
高影响因子
Inorganic Chemistry Frontiers
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2026
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IF 6.2
siqing Wang,Yan Zhang,Pengda Xiang,Dawei Chen,Qiling Li,Zhiyan Guo,chen chen
Electrocatalytic urea synthesis from CO2 and NOx offers a sustainable route for chemical production and environmental remediation. While grain-boundary engineering has emerged as a promising strategy to accelerate the sluggish kinetics of C–N coupling, whether it can simultaneously regulate the reaction pathways of both carbon and nitrogencontaining molecules remains unclear. Hence, we employed single-active-site TiO2 as a model catalyst and constructed polycrystalline grain boundaries to boost both the activity and selectivity of urea synthesis. Atomic-scale structural inducers (Fe) served as nucleation nodes for grain-boundary formation and promote the generation of abundant oxygen vacancies, which captured and locally concentrated electrons to facilitate the adsorption, activation, and C−N coupling of key reaction intermediates. Operando electrochemical impedance spectroscopy demonstrated enhanced interfacial charge transfer and faster interfacial response frequencies. In situ infrared spectroscopy directly tracked the adsorption and activation of both reactants as well as the formation of the critical C–N bond. This work provides a general design principle for developing advanced electrocatalysts for efficient C–N coupling.
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高影响因子
Catalysis Science & Technology
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2026
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IF 4
Kaiyang Lian,Fei Li,Lijuan Ma,Ranran Wu,Zhiguang Zhu
Glycine, the simplest amino acid with versatile physiological functions, is widely used in pharmaceuticals, animal feed, and the food industry. However, conventional production methods are limited by sustainability, safety, and environmental concerns. Here, we develop an efficient and green one-pot in vitro multi-enzyme cascade that converts oxalate into glycine under mild conditions. Upon optimization of the reaction conditions and integration of a cofactor recycling system, nearly complete conversion (100%) of oxalate to glycine was achieved in a 1-mL reaction system within 7 hours. After 4 hours of reaction in a 10 mL system, the glycine yield reached 95.7%, with a corresponding synthesis rate of 179.6 mg L-1 h-1. This work demonstrates that a C2-fixing multi-enzyme cascade circumvents the inherent challenge of C-C bond formation, achieving efficient conversion of CO2-derived oxalate to glycine, and presents a practical and conceptually innovative strategy for carbon-negative chemical synthesis.
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高影响因子
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