JOURNAL OF APPLIED POLYMER SCIENCE
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2024
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IF 2.7
Wei Zhao,Hongjing Liu,Chengpeng Zhang,Yuyang Cao,Yuying Xu,Xueli Liu,Zhen Lu
Metal–organic frame UiO-66-NH 2 was modified by 3-glycidyl ether oxypropyl trimethoxysilane (KH560), and KH560-UiO-66-NH 2 was synthetized and added to Pebax to prepare KH560-UiO-66-NH 2 /Pebax mixed matrix membranes (MMMs). The epoxy group of KH560 had an amine-epoxidation reaction with the NH 2 in UiO-66-NH 2 , which prevented UiO-66-NH 2 from agglutinating in the MMMs. In addition, the N H bond and OH bond of KH560-UiO-66-NH 2 could theoretically form hydrogen bonds with CO and N H bonds in the main chain of polymerization, respectively, so as to improve the interfacial compatibility between fillers and polymers. The structure and properties of the filler particles and MMMs were evaluated by Fourier transform infrared spectrometer, x-ray diffraction, scanning electron microscopy, and thermogravimetric analyzer. The results showed that the filler particles were successfully synthesized, and had good crystallinity, uniform size distribution, and good thermal stability. The inorganic and organic interfaces of MMMs had no obvious interface defects. The obtained KH560-UiO-66-NH 2 /Pebax MMMs showed CO 2 permeability of 111.52 Barre and CO 2 /N 2 selectivity of 92.16, which were 85.65% and 88.73% higher than that of pristine membranes, respectively. The gas separation performance of MMMs was significantly improved, exceeding the upper bound of 2008 Robeson.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xueru Zhao,Jinlong Wu,Jiaxin Bai,Ting Zhang,Zhenli Lv,Maoxu Wang,Min Zhu,Jing Li,Feng Li
Cuprous oxide (Cu 2 O) is a promising material for photoelectrocatalytic CO 2 reduction (PEC-CO 2 RR); however, its widespread application is hindered by issues such as photocorrosion, structural instability, and low selectivity toward desirable products. In this work, a Cu 2 O-BiOBr nanohybrid catalyst with excellent visible light responsiveness are successfully developed using energy band structure matching and morphology modulation strategies. This heterostructure exhibits a three-dimensional bridge-like architecture composed of interwoven one-dimensional nanorods and two-dimensional nanosheets. Cu 2 O acts as a surface electron-rich active center, while BiOBr functions as both a co-catalyst and photogenerated electron storage, enabling efficient photoelectrocatalytic conversion of CO 2 under visible light irradiation. That is, the optimized Cu 2 O-BiOBr-2 catalyst achieves a C 2+ Faraday efficiency (FE) of 51% at −0.6 V vs. RHE, which is 2.55 times exceeding the pure Cu 2 O catalysts, The findings obtained from in-situ spectroscopic characterization reveal that the efficient transport channel of the constructed heterojunction enhances charge transfer efficiency at the catalyst interface and boosts redox capacity, improving both efficiency and stability of Cu 2 O in PEC-CO 2 RR. This work provides new insights for constructing novel heterojunctions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Linglong Wang,Bangyan Zhang,Yang Song,Tao Gan,Jiansong Miao,Peng Zhang,Jingjing Jiang,Chunming Xu,Xiaohui Sun
Nitrogen-doped carbon nanoparticle-supported single-iron-atom catalysts (denoted as Fe-N-C) have been widely investigated in the electrocatalytic CO2 reduction reaction (CO2RR). However, for most Fe-N-C catalysts fabricated via high-temperature pyrolysis, abundant active Fe sites are buried in the bulk of microporous carbon substrate, with poor accessibility. The morphology limitation immensely alleviates the exposure of active sites at the critical three-phase interfaces and hinders the mass transfer of reactant molecules within electrodes. Herein, we present a facile soft-template coating approach to fabricate a core–shell Fe-N-C catalyst with highly accessible Fe sites at the surface by pyrolysis of an iron-coordinated polydopamine-coated ZIF-8 composite precursor. The unique core–shell structure of Fe-N-C shortens the diffusion path of ions and CO2, and it facilitates CO product elimination. Such an electrode assembly significantly boosts the electrocatalytic CO2RR in a gas-diffusion-electrode with a CO Faradaic efficiency (FECO) of ∼97% at an industrial current density of 100 mA/cm2. This work sheds light on the synthesis of single-atom catalysts with highly accessible active sites in surface layers for the CO2RR and other electrocatalytic reactions with high activity and efficient mass transport.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Zhi-Wen Wang,Qiang Wan,Ying-Zhang Shi,Huan Wang,Yue-Yue Kang,Shu-Ying Zhu,Sen Lin,Ling Wu
Ultrathin TiO 2 nanosheet (NST) with abundant Ti 3+ sites is developed as a photocatalyst which exhibits a high yield (147.2 μmol g −1 h −1 ) and selectivity (96.8%) for CO 2 to CH 4 . The results of in situ FTIR, in situ EPR and density functional theory (DFT) calculation suggest that CO 2 would be selectively activated on NST surface via forming the bridging Ti···CO 2 − ···Ti coordination species which not only lowers the activation energy barrier, but also determines the selectivity of CH 4 . Additionally, NST with the better separation and transfer ability for photogenerated electrons-holes can fleetly supply the electrons to CO 2 molecules for high efficiently producing CH 4 via the Ti-C coordination bond. Finally, a possible mechanism of the synergistic effect about coordination-activation and photocatalysis is discussed at a molecule level. This work would offer a perspective for designing an effective photocatalyst and tailoring the selectivity of products by coordination activation.
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ADVANCED MATERIALS
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2025
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IF 26.8
Zailun Liu,Yunfei Ma,Junqing Li,Ying Tu,Hui Yang,Kelin He,Chao Chen,Yulin Wang,Xiang Lin,Hongli Sun,Chenliang Su,Qitao Zhang
Uncovering the excitation processes of photocatalysts and enhancing the dissociation of excitons into free photogenerated electrons and holes for photocatalytic CO 2 reduction is imperative yet quite challenging. Herein, an efficient strategy of reducing the binding energy of excitons to boost exciton dissociation is reported by anchoring the low valence single-atom Cu sites in In 2 S 3 nanosheets (Cu-In 2 S 3 ), which can enhance photocatalytic CO 2 reduction activity. The investigations of photo-irradiated Kelvin probe force microscopy (KPFM), in situ irradiates X-ray photoelectron spectroscopy (XPS), and temperature-dependent photoluminescence (TD-PL) indicate that the doping of low valence single-atom Cu can efficiently drive the charge transfer and separation. Moreover, the studies of the dynamic behaviors of charge carriers by femtosecond time-resolved spectroscopy (fs-TAS) reveal that the doping of low valence Cu single-atom sites allows the promotion of exciton dissociation by reducing the binding energy of the exciton, resulting in an enhanced photocatalytic CO 2 reduction of Cu-In 2 S 3 nanosheets. The aforementioned strategy for enhancing the dissociation efficiency of excitons in photocatalysts will offer a highly efficient and promising approach for the photocatalytic CO 2 reduction and other photocatalytic applications.
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PubMed
高影响因子
Science Bulletin
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2025
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IF 21.1
Wanguo Gao,Zhe Lu,Yecheng Leng,Chengyang Wu,Yingfang Yao,Xi Zhu,Junchuan Sun,Xiwen Yu,Cheng Wang,Congping Wu,Wenlei Wu,Bing Wang,Lu Wang,Zhigang Zou
Cu-based catalysts attract considerable attention because of their exceptional CO 2 photo-/electro-/thermo-reduction capacities, where Cu(I) is generally treated as the active species. However, a significant problem hindering the large-scale applications of Cu-based catalysts is the inactivation of Cu(I) via irreversible redox to Cu(II)/Cu(0). This study proposes a Cu(I) valence pinning method based on hydroxyapatite (HAP). Experimental and theoretical studies demonstrate that the phonon resonance among the Cu(I) ions, their adjacent heteroatoms, and the intermediates adsorbed at the Cu(I) sites yields Cu(I) valence electrons in their lowest energy states. Thus, Cu(I) is stabilized, stable, and efficient photothermal CO 2 hydrogenation is promoted. However, because of the change of Cu(I) coordination environment during the CO 2 hydrogenation reaction, Cu(I) ions migrate into the bulk phase, leading to activity attenuation. Nevertheless, Cu(I) ions can be pulled out to the surface of HAP under the oxidative humid air condition, and the catalytic activity can be easily recovered. Thus, we propose a simple cyclic reaction/regeneration process. This enables the Ca 5 (FeCuCe) 5 -HAP catalyst to achieve the CO yield of 402.8 mmol g −1 h −1 and a CO 2 conversion rate of 27.7%, which is close to the thermodynamic equilibrium. This catalyst also displays a selectivity of approximately 100% and cycle stability of 156 h at 500 °C under a pressure of 1 atmospheric. Our study provides a viable method for the scale applications of Cu(I) based catalysts in the “negative carbon” industries.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Shuzhuang Sun,Bocheng Yu,Weiwen Meng,Yongqing Xu,Yanmei Shen,Zhehao Sun,Zongyou Yin,Hongman Sun,Hui Zhou,Hengshan Qiu
Understanding the dynamic phase change under operational conditions is crucial for the development of high-performance catalysts. Ni-based alloys have long been elucidated as active and selectivity-tunable phases in CO 2 hydrogenation, while their gas-dependent surface reconstruction and correlation with dynamic activities, particularly under gas-swing catalytic conditions, remain poorly understood. Herein, we demonstrate that Zn can segregate from the NiZn alloy in a CO 2 atmosphere enabling formation of well-dispersed surface Ni atoms that can gradually homogenize back into the alloy under H 2 . Consequently, formation of highly stable intermediates, bridged and multi-centered carbonyls, can be effectively avoided due to the absence of closely-packed Ni sites. Instead, the linear carbonyls on Ni undergo desorption rather than further hydrogenation due to their relatively low binding energy, rendering a high CO selectivity. This insight of gas-dependent evolution of sites will enable the rational design of alloy catalysts for multi gas swing catalytic applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Ming-Dong Xie,Jia-Meng Sun,Zhong-Hua Zhang,Hong-Qing Liang,Zhi-Kang Xu
Electrochemical CO 2 reduction (CO 2 RR) in acidic media circumvents carbonate crossover and salt precipitation inherent to alkaline and neutral systems, but suffers from low selectivity due to the dominance of hydrogen evolution. While alkali cations suppress proton activity, they inevitably lead to catastrophic (bi)carbonate deposition and electrode flooding. Here, we decouple CO 2 RR from alkali cations by constructing a micro-alkaline catalytic environment using a proton-blocking hydrophobic membrane with tethered cations. We designed a series of quaternized copolymers from dimethylaminoethyl methacrylate and lauryl methacrylate (qDMA-n), where the “cation–hydrophobicity balance” was precisely tuned to optimize the balance between Donnan exclusion and water management. Integrated into a zero-gap membrane electrode assembly electrolyzer, the optimized membrane enabled CO 2 RR on Ag catalysts with a CO faradaic efficiency of 96.9 % and a single-pass conversion efficiency of 92.4 % at 200 mA cm⁻ 2 in pure 0.05 M H 2 SO 4 , maintaining stable operation for over 100 h. Finite element simulations, rotating disk electrode tests and in-situ Raman spectra revealed that the balance between cationic and hydrophobic domains plays a key role in forming a stable micro-alkaline interface despite bulk acidity, leading to effective HER suppression. This work provides a practical and generalizable interface design principle for efficient CO 2 electrolysis in strong acids, offering new opportunities for durable, high-efficiency CO 2 electrolyzers without alkali cations.
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ENERGY & FUELS
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2025
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IF 5.3
Guang Miao,Pengxian Ye,Junyang Wang,Jiawu Huang,Jing Xiao,Chunshan Song
The development of cost-effective, high-performance sorbents for CO2 capture in hydrogen purification remains a critical challenge, particularly under industrial conditions of ultralow CO2 concentrations and ambient temperatures. This study systematically investigates polyethylenimine (PEI)-impregnated SiO2 and SBA-15 sorbents, with a focus on enhancing CO2 uptake and kinetics through polyethylene glycol (PEG) incorporation. Although PEI-SBA-15 sorbents showed higher static and dynamic CO2 uptakes compared to PEI-SiO2 sorbents, its diffusion barrier lowers the adsorption rate in the flow system. The poly(ethylene glycol) (PEG) polymers were introduced to PEI-SiO2 to improve the mass transfer of CO2 in PEI clusters. The low PEI loading was found to be beneficial to CO2 adsorption on SiO2, resulting in superior CO2 uptakes and a lower diffusion barrier than PEI-SBA-15 sorbents. The characterization was conducted to uncover physical and chemical properties. The breakthrough experiments of PEI-30-SiO2 with PEG derivates confirmed that the O in the skeleton of PEG played an important role in the interaction between PEI and PEG rather than terminal OH groups. This work also demonstrated the CO2 desorption and stability of PEG-modified PEI-SiO2 sorbents in H2.
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Journal of Physical Chemistry C
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2025
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IF 3.2
Chuyi Zhang,Jiaxin Liu,Zhi Sun,Yuning Liang,Qun Xu
With the development of spintronics, ferromagnetic nanomaterials have shown unique advantages in the fields of information storage and quantum computation. The ABO3-type perovskite oxide ZnSnO3 is expected to realize d0 ferromagnetism due to its tunable crystal structure and unique electron arrangement. In this work, for the first time, the inhomogeneous oxygen octahedral structural distortion along the c-axis induced by SC CO2 can be found in 2D ZnSnO3, i.e., distortion of ZnO6 is larger than that of SnO6, and they are served as the structural basis for the generation of room-temperature ferromagnetism. In addition, combining the change in the concentration of the oxygen vacancies to ultimately realize the room-temperature d0 ferromagnetism in ZnSnO3 (Tc = 400 K, Ms = 0.1123 emu/g) can be presented. Therefore, this study establishes a new strategy for the development of transition metal-free ferromagnetic materials for the application of spintronic devices at room temperature.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Shuai Yue,Guobin Xiao,Qiujin Shi,Xijiao Mu,Manke Zhang,Mingzheng Xie,Jing Cao
As a promising technology with both environmental and economic benefits, photocatalytic CO 2 conversion relies heavily on photo-carrier transport properties. However, oxide photocatalysts often face a significant limitation due to their restricted carrier transport distances, typically below 100 nm. Here, a surface electric field regulation strategy is proposed that enhances carrier transport in metal oxide photocatalysts by integrating specific porphyrin supramolecular assemblies. Through spin-coating, monoamine metal porphyrin assemblies are uniformly deposited on the BiVO 4 photocatalyst via van der Waals interactions. The electronic coupling between amine groups and Co atoms in adjacent porphyrin units generates unoccupied orbitals, which facilitate the accumulation of holes within the Co-porphyrin supramolecular system. This coupling induces interfacial electron redistribution and charge density reorganization, creating an intense surface electric field on BiVO 4 with an intensity of 17.4 V m −1 . As a result, the mobility of photo-carriers within BiVO 4 is significantly enhanced, extending the hole diffusion length from 46.7 to 232.9 nm and enabling more efficient charge extraction at the surface. This improvement results in a 7.3-fold increase in the photocatalytic CO 2 reduction performance, achieving an external quantum efficiency of 1.86%. The proposed approach offers a generalizable method for enhancing photo-carrier properties in photocatalytic systems.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Qi Tan,Zhiwei Liu,Yao Zhang,Yongle Xia,Xiaoyi Zhang,Bingliang Gao
Efficient recovery of CO 2 from industrial flue gas and its subsequent resource utilization have gained significant attention in recent years due to growing environmental and energy concerns. In this paper, a series of ternary vitreous mixture solvents (VMSs) composed of a superbase-alcohol system and functional additives, such as succinimide (Suc), n-hydroxysuccinimide (HOSu), and 2-imidazolidinone (IM), were synthesized for CO 2 capture. The effects of various additives on both the CO 2 capture capacity and the physicochemical properties of the system were systematically investigated. Among the systems tested, 1,5-diazabicyclo[4.3.0]non-5-ene (DBN)−Methanol (MeOH)−Suc (1:1:0.1) exhibited the highest absorption performance, achieving an absorption capacity of 0.274 g CO 2 /g VMS at 25℃ and 1 bar. Notably, the DBN−MeOH−Suc VMS maintained a CO 2 removal efficiency exceeding 90 % even under a low CO 2 partial pressure corresponding to a volume concentration of 1.7 %. Furthermore, nearly complete CO 2 desorption was achieved within 15 min at 60℃ under a nitrogen atmosphere. A CO 2 absorption mechanism was proposed based on NMR and FTIR spectroscopic investigations, as well as quantum chemical calculations. The results suggest that both deprotonated alcohols and additives synergistically participate in CO 2 capture. The VMSs developed in this work offer multiple advantages, including simple synthesis, high CO 2 absorption and desorption kinetics, low post-absorption viscosity, low desorption temperature, and excellent recyclability. These features collectively provide an innovative pathway for the advancement of next generation CO 2 absorbents.
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