APPLIED CATALYSIS A-GENERAL
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2024
·
IF 4.7
Meidan Que,Yabo Wang,Ruochen Shi,Xun Sun,Jun Xu,Peihong Ma,Yanbo Sun,Jing Guan,Shengxia An
MIL-125(Ti) is well known for having stable structure, tunable electron structure, and multiple active sites, which is commonly studied in the field of photocatalysis . In this work, a series of rare earth (RE) doped MIL-125(Ti) (RE=Ce, Pr, Tm, Dy, Eu, and Sm) are prepared via the one-step hydrothermal method . Notably, Pr-MIL-125 displays a significantly enhanced catalytic performance than other RE-doped MIL-125, resulting in a maximal CO and CH 4 yield of 13.30 and 0.87 µmol·g −1 ·h −1 , respectively, which are 2.53-fold and 4.14-fold of the pristine MIL-125. The layered morphology endows Pr-MIL-125 with more active sites and facilitates the reaction of photoreduction CO 2 . Furthermore, the promoted photoactivities attributed to Pr ion dopant can act as electron transfer bridge and suppress charge recombination. This work would provide insight and guidance for designing RE-MOF based photocatalysts and enhancing the performance of photoreduction CO 2 .
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 14
·21267-21278
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IF 0
Zhao Dongling,Geng Linlin,Jia Yanfei,Wei Jianwen,Zhou Xiaobin,Liao Lei
High-temperature solid adsorbent Li 4 SiO 4 has received broad attention due to its high theoretical adsorption capacity, high regeneration capacity, and wide range of raw materials for preparation. In this paper, a Li 4 SiO 4 adsorbent was prepared by MCM-48 as the silica precursor and modified by doping with metal ions (Ca 2+ and Na + ) for high-temperature capture of low-concentration CO 2 . The results showed that the surface of the Ca-doped (or Na-doped) Li 4 SiO 4 adsorbent developed some particles that are primarily composed by Li 2 CaSiO 4 (or Li 3 NaSiO 4 ). Furthermore, the grains of the adsorbents became finer, effectively increasing the specific surface area and enhancing adsorption performance. Under 15 vol% CO 2 , the maximum CO 2 adsorption was 25.63 wt% and 32.86 wt% when the Ca 2+ doping amount was 0.06 and the Na + doping amount was 0.12, respectively. These values were both higher than the adsorption capacity before the metal ion doping. After 10 adsorption/desorption cycles, the adsorption capacity of Na-doped Li 4 SiO 4 increased by 9.68 wt%, while that of Ca-doped Li 4 SiO 4 decreased by 7.98 wt%. This difference could be attributed to the easy sintering of the Ca-containing adsorbent. Furthermore, a biexponential model was used to fit the CO 2 adsorption curve of the adsorbent in order to study the adsorption kinetics. Compared to the conventional Li 4 SiO 4 , the Ca/Na-doped adsorbent offers several advantages, such as a high CO 2 adsorption capacity and stable cycling ability.
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PROGRESS IN ORGANIC COATINGS
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2023
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IF 6.6
Zhenhong Huang,Chaozhi Wang,Hualin Li,Jiaoyan Ai,Lina Song,Baohua Liu
Brushable polyurea based on slow reactive process was prepared by simple, mild and solvent-free method. Firstly, polyurethane prepolymer was synthesized from poly (propylene carbonate) diol (PPCD, copolymer of propylene oxide/CO 2 ) and 4,4′-dicylocyhexylmethane diisocyanate (HMDI). Polyurethane-urea (PPCD–PUU) was then obtained by the chain extension of prepolymer with polyaspartic ester (PAE). The mechanical properties of PPCD–PUU were optimized by adjusting the content of –NCO in the prepolymer and the ratio of prepolymer to PAE. The mechanical strength , thermal resistance, solvent resistance and hydrolysis resistance of PPCD–PUU were compared with those of PUUs derived from polypropylene glycol and poly-caprolactone diol. The results showed that the comprehensive mechanical properties of PPCD–PUU were balanced when the R value was 1.15 and the content of –NCO was 8 %. The tensile strength was 20.5 MPa, the elongation at break was 352 %, and the Young's modulus was 168.2 MPa. Especially, after soaking in 10 % H 2 SO 4 aqueous solution, 10 % NaOH aqueous solution and 10 % NaCl aqueous solution for 24 h, the tensile properties were basically unchanged. Manual applied polyurethane-urea based on commercial PPCD has broad application prospects because it avoids the use of expensive spraying equipment.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2017
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IF 6.035
Xiao-Min Zhang,Zhuo-Heng Tu,He Li,Lei Li,You-Ting Wu,Xing-Bang Hu
In this work, four diamine-monocarboxylate-based protic ionic liquids (PILs) were firstly introduced to prepare supported ionic liquid membranes (SILMs) and the selective separation of CO 2 /N 2 and CO 2 /CH 4 gas pairs in these SILMs under humidified condition were investigated. The effects of transmembrane pressure and temperature on the permeablity of CO 2 and the permselectivity of CO 2 /N 2 and CO 2 /CH 4 gas pairs were also studied. It is found that the supported PILs with 15 wt% water exhibit much higher CO 2 permeabilities under humidified conditon than those pure PILs under dry condition. The permeability increases with the decreasing transmembrane pressure, indicating a typical feature of facilitated transport membrane . The permeability of CO 2 increases with the increasing temperature whereas the permselectivity of CO 2 /N 2 and CO 2 /CH 4 decreases at the same time. The highest CO 2 /N 2 selectivities obtained is 151, and the highest CO 2 /CH 4 selectivities is 72. These PILs is found to be tunable and selective carriers of CO 2 in the presence of water, and the supported protic-ionic liquid membranes exhibit competitive permeability and higher permselectivity in comparison with the supported aprotic- ionic- liquid membranes.
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高影响因子
DYES AND PIGMENTS
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2014
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IF 3.468
Huanqing Cui,Hui Liu,Si Chen,Ruimeng Wang
An amphiphilic spiropyran-based random copolymer containing methacrylic acid unit has been prepared and investigated with obvious negative solvatochromism in five different solvents. It was found that the polarity of comonomer influenced the photochromic behavior of spiropyran. The synthesized copolymer exhibited a good reversible behavior in aqueous solution: the addition of strong acid promoted the isomerization from spiropyran (SP) to merocyanine (MC), and the inverse process was achieved by the introduction of strong base. Much more importance, the effect of comonomer was utilized for the selective Co 2+ recognition. The locations of the maximum absorption peak stay almost as same as MC when it is complexed with Cu 2+ , Mn 2+ and Hg 2+ . The location, however, moves from 551 nm to 526 nm upon complexation with Co 2+ . The obvious color change of the solution from purple to claret-red after complexation with Co 2+ was observed. This interesting phenomenon is practically convenient for the visual recognition of Co 2+ .
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Jingxing Cheng,Kun Zhu,Houfang Lu,Hairong Yue,Changjun Liu,Bin Liang,Siyang Tang
CO2 emissions reduction has become a hot issue to relieve global warming in recent years. CO2 absorption with amines aqueous solutions is a promising method for its capture, and increasing CO2 capacity and reducing energy consumption are essential for its application. In this work, a data set of 29 different amines was regressed with genetic function approximation (GFA) and artificial neural network (ANN) algorithm to find a predictive quantitative relationship between amine structure and CO2 absorption capacity. Density functional theory (DFT) methods at levels B3LYP and 6-311+g (d,p) were used to optimize the structures. Both reactants and products were introduced in regression, and an optimal model with best relevance and predictability for CO2 absorption at 313 K was obtained and experimentally confirmed. Descriptors analysis showed that reducing the number of hydroxyl groups, increasing molecular mass, and changing steric effect of amine structure would increase its CO2 absorption capacity. Two new amine structures predicted with high absorption capacity were proposed.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2016
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IF 5.393
Shufeng Shen,Ya-nan Yang,Yangyang Bian,Yue Zhao
Aqueous amino acid salts are considered as an attractive alternative to alkanolamine solvents (e.g., MEA) for carbon dioxide (CO2) absorption. The kinetics of CO2 into unloaded aqueous solutions of potassium lysinate (LysK) was studied using a wetted wall column at concentrations ranging from 0.25 to 2.0 M and temperatures from 298 to 333 K. Physicochemical properties of aqueous LysK solutions such as density, viscosity, and physical solubility of CO2 were measured to evaluate the reaction rate constants. The reaction pathway is described using zwitterion mechanism taking into account the effect of ionic strength on the reaction rate. Under the fast pseudo-first-order regime, the reaction rate parameters were obtained and correlated in a power-law reaction rate expression. LysK shows higher chemical reactivity toward CO2 than the industrial standard MEA and most of amino acid salts. Its reaction rate constants increase considerably with concentration and temperature. The reaction order is found to be an average value of 1.58 with respect to LysK. The forward second-order kinetic rate constant, k20, are obtained as 31615 and 84822 m3 kmol–1 s–1 at 298 and 313 K, respectively with activation energy of 51.0 kJ mol–1. The contribution of water to the zwitterion deprotonation seems to be more significant than that of LysK for the above-mentioned kinetic conditions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Min Sun,Zhenni Wang,Xin Qian,Ziyong Liu,Fengjie Wu,Hanlei Sun,Hongzhi Wang,Zaiping Guo,Licheng Liu
The CuO/Ga 2 O 3 –550 catalyst achieves a high CH 4 Faradaic efficiency of 72.1%. • Hydroxyl-rich Ga 2 O 3 support modulates interfacial proton delivery. • Surface hydroxyls accelerate H 2 O dissociation and lower the *CO 2 − to *COOH energy barrier. • Hydroxyl-mediated water activation and *CO stabilization contribute to deep methanation. Electrochemical reduction of CO 2 (CO 2 RR) to methane (CH 4 ) provides a sustainable pathway for the green and efficient CO 2 conversion, yet it is hindered by the competing hydrogen evolution reaction and poorly regulated interfacial proton microenvironments. This work establishes hydroxyl-content modulation on gallium oxide (Ga 2 O 3 ) supports as a robust strategy for CuO/Ga 2 O 3 catalyst fabrication and CO 2 RR to CH 4 optimization. Notably, the CuO/Ga 2 O 3 –550 catalyst with a moderate hydroxyl content exhibits excellent performance, achieving a Faradaic efficiency of 72.1% at −1.5 V vs. RHE for CH 4 production. The kinetic isotope effect (KIE) result reveals that surface hydroxyl groups significantly accelerate *H transfer dynamics. In situ spectroscopy and DFT calculations clarify that surface hydroxyl groups on Ga 2 O 3 not only promote the CO 2 reduction pathway by lowering the energy barrier for CO 2 -to-*COOH conversion, but also optimize *CO adsorption on Cu sites and stabilize *CHO intermediates. Moreover, hydroxyl-mediated water molecular activation reduces the energy barriers for H 2 O dissociation, generates abundant active hydrogen groups, thereby promotes proton-coupled electron transfer toward deep methanation. This study underscores the great potential of support hydroxyl engineering to regulate local proton environments for the selective electroreduction of CO 2 to CH 4 . Surface hydroxyl groups on Ga 2 O 3 regulate the local interfacial microenvironment around Cu active sites and promote H 2 O dissociation, thereby providing accessible proton sources for CO 2 electroreduction. The hydroxyl-mediated proton delivery mechanism facilitates proton delivery on Cu sites, increases *CO coverage, promotes the formation of the *CHO intermediate, and suppresses the competing HER process. Download: Download high-res image (175KB) Download: Download full-size image
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123938
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IF 7.5
Yanli Wang,Wenqing Xu,Tingyu Zhu,Zhikun Zhang
The severe self-aggregation and instability of polyamines at high loadings remain major mass-transfer limitations in solid amine sorbents. To overcome this kinetic limitation, we propose a molecular-level regulation strategy by incorporating trace Ni (1 wt%) into tetraethylenepentamine (TEPA) confined within a hierarchical porous geopolymer-zeolite framework. Rather than acting as a conventional promoter, the intentionally introduced Ni forms specific Ni-TEPA coordination complexes, which significantly disrupted the intermolecular hydrogen-bonding network and inhibited polyamine aggregation. Consequently, the Ni-modified sorbent effectively alleviated diffusion resistance, exhibiting substantially improved amine accessibility and accelerated adsorption kinetics. Density functional theory (DFT) combined with spectroscopic analyses revealed that Ni coordination systematically reduced the electron density around the amine nitrogen sites, substantially lowering the apparent adsorption activation energy to 8.28 kJ/mol. Under simulated post-combustion conditions (15 vol% CO 2 , 70 °C), the optimized sorbent achieved a high CO 2 uptake of 3.92 mmol/g and retained 99.75% of its initial capacity after 10 cycles. Furthermore, utilizing waste-derived zeolite-geopolymer (from municipal solid waste incineration and coal fly ash) as the robust support yields a potentially attractive manufacturing cost of 158.99 ¥/kg, providing a sustainable and scalable chemical engineering approach for industrial flue gas treatment.
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高影响因子
CHEMPHYSCHEM
·
2026
·Vol. 27
·期 14
·e70511
·
IF 2.4
Zezong Zhao,Xiaoyang Fan,Haimin Xu,Guihua Hu,Jiancheng Tong,Sheng Zhang,Yukun Gao,Penggang Yin
By pyrolyzing Cu‐based MOFs, a Cu 0 /Cu +1 /C/N catalyst with a porous carbon layer coating was synthesized. The combination of the Cu ion‐rich active sites derived from MOFs and the Raman signal enhancement associated with Cu nanostructures and charge–transfer interactions, which contributes to the SERS effect, was utilized for in situ investigation of the electrochemical CO 2 reduction reaction (CO 2 RR) process. This study focuses on the catalytic performance and reaction mechanisms of Cu‐MOF‐derived materials in the electrocatalytic CO 2 reduction reaction, using in situ Raman and SERS techniques for real‐time monitoring and characterization. The results indicate that Cu‐MOF‐derived materials significantly enhance the selectivity toward C 2 products by tuning the valence state distribution of copper (Cu(I)/Cu(0)) and the structure of active sites. Moreover, the porous carbon‐coated Cu elements exhibit stable catalytic performance during the electrocatalytic process (inhibiting hydrogen evolution reaction and stabilizing the valence state of Cu ions). In addition, in situ spectroscopy reveals the dynamic evolution of key intermediates (such as *CO and *CHO) and the ion adsorption process on the catalyst surface, providing crucial insights into the catalytic behavior of Cu‐MOF‐derived materials. We synthesized a Cu 0 /Cu + /C/N catalyst with a porous carbon coating by pyrolyzing Cu‐based MOFs. The abundant Cu‐ion active sites inherited from the MOF structure and the electromagnetic‐field–enhanced charge‐transfer effect of the carbon matrix enable strong SERS activity for in situ monitoring of the CO 2 reduction reaction (CO 2 RR). Using in situ Raman and SERS, we investigated the catalytic performance and reaction mechanism of Cu‐MOF‐derived materials. The results show that regulating the Cu 0 /Cu + valence distribution and tuning the active‐site structure significantly enhance C 2 product selectivity. The porous carbon layer further stabilizes Cu species and suppresses the competing hydrogen evolution reaction, ensuring durable catalytic performance. In situ spectroscopy reveals the dynamic evolution of key intermediates (*CO, *CHO) and ion‐adsorption behavior on the catalyst surface, providing critical mechanistic insights. This work highlights the potential of MOF‐derived Cu catalysts for efficient CO 2 RR and offers guidance for designing advanced electrocatalysts.
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PubMed
高影响因子
POLYMER
·
2026
·
IF 5.1
Xu Jiang,Wenwen Jiang,Xinqi Xie,Xinyi Shen,Yu Tang,Chen Wang,Huanwang Jing,Faliang Gou
Three monoimidazole-modified cobaltoporphyrins with different substitution positions were designed and synthesized as bifunctional homogeneous catalysts for the alternating copolymerization of propylene oxide (PO) and CO 2 to produce biodegradable poly(propylene carbonate) (PPC) under mild conditions without a cocatalyst. Their catalytic performance strongly depends on the ligand skeleton, which determines product selectivity. Under optimal conditions, catalyst X- o 4 showed high PO conversion, polymerization selectivity, high molecular weight polycarbonate, and narrow molecular weight distribution. Kinetic studies using X- o 4 and bisimidazole-modified J- o 4 gave apparent activation energies for polycarbonate and cyclic carbonate. Based on structural and experimental data, a competition mechanism between polymerization and cycloaddition is proposed. Density functional theory (DFT) calculations support this mechanism, explaining the temperature-dependent selectivity and the different behaviors of mono- and bis-imidazole catalysts.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Huilin Li,Xuechong Ding,Teng Zhou
Reducing regeneration energy remains a central challenge in post-combustion CO 2 capture by chemical absorption. In this work, nine aqueous MDEA/DMEA/PZ blends were systematically screened using thermodynamic performance indicators, including the heat of absorption, heat capacity, and equilibrium CO 2 absorption capacity. Two formulations, D30P10 (30% DMEA +10% PZ) and M5D25P10 (5% MDEA +25% DMEA +10% PZ), were identified as the most promising candidates for achieving low regeneration energy. These two solvents were further evaluated against two benchmarks, 30 wt% MEA and M30P10 (30% MDEA +10% PZ), in cyclic absorption–desorption experiments. Among them, M5D25P10 delivered the best overall balance of stable cyclic performance and a cyclic capacity about 0.55 mol CO 2 /mol amine. Benefiting from its high cyclic capacity and low heat of absorption, this solvent achieved a regeneration energy of 2.98 GJ/t CO 2 , which was 21.2% and 4.5% lower than those of 30 wt% MEA and M30P10, respectively. Kinetic performance indicators, including the initial absorption rate ( r abs ini ) and the overall mass transfer coefficient ( K G ), were also evaluated, and M5D25P10 exhibited the highest mass transfer coefficient among all tested solvents. These results collectively confirm that M5D25P10 is a highly promising solvent for post-combustion CO 2 capture. Moreover, a robust empirical correlation between r abs ini and K G was established for the first time, providing a rapid and solvent-efficient means of estimating mass-transfer performance.
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高影响因子
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