ChemistrySelect
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2024
·Vol. 9
·期 40
·e202400345
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IF 1.9
Bo Pei,Dongdong Chu,Jiajia Huang
Graphical Metal ions modified azo-linked porous polymers for CO 2 capture through coordination adsorption with high adsorption capacity and excellent cycling stability. Herein, a novel CO 2 adsorption materials (ALP−M) with controllable adsorption heat were prepared by loading metal ions on azo-linked porous polymer through coordination interaction. The as-prepared ALP−M showed excellent CO 2 capture performance with a column adsorption capacity 4.99 mmol g −1 at 273 K (1 bar) and 98 % capacity retention rate after 500 adsorption and desorption cycles. Porous polymer show great potential for CO 2 capture owing to its high specific surface area, adjustable porous structure and chemical structure. Herein, a novel CO 2 adsorption materials ALP−M (M: Cu 2+ , Mg 2+ , Ni 2+ ) were prepared through coordination between azo-linked porous polymer (ALP) synthesized by oxidative coupling polymerization of tris(4-aminophenyl)amine and metal ions. The structures and morphology of as-prepared materials were demonstrated by FT-IR, XRD, XPS, BET and SEM, the CO 2 capture performance and mechanism of ALP−M were also investigated through static adsorption and column adsorption experments, the results show that metal ions can enhance the CO 2 adsorption and desorption performance of ALPs by coordination adsorption. ALP−M showed a highest static CO 2 adsorption capacity of 2.67 mmol g −1 at 273 K (1 bar), which is 35.5 % higher than that of ALP. The metal ions served as Lewis acid sites can enhance the affinity of adsorbent for CO 2 . In column adsorption experiments, the ALP−M showed a higher saturated adsorption capacity 4.99 mmol g −1 at 273 K (1 bar) than that of static adsorption, and excellent cycling stability after 500 adsorption and desorption cycles, the adsorption capacity retention rate of ALP−M for CO 2 can reach 98 %.
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Advanced Science
·
2024
·
IF 14.3
Jia Shi,Andrew J. Tanentzap,Yuanze Sun,Jianjun Wang,Baoshan Xing,Matthias C. Rillig,Changchao Li,Ling Jin,Fang Wang,Tanveer M. Adyel,Jianying Shang,Xiang Wang,Jie Wang
Microplastic pollution in terrestrial ecosystems threatens to destabilize large soil carbon stocks that help to mitigate climate change. Carbon-based substrates can release from microplastics and contribute to terrestrial carbon pools, but how these emerging organic compounds influence carbon mineralization and sequestration remains unknown. Here, microcosm experiments are conducted to determine the bioavailability of microplastic-derived dissolved organic matter (MP-DOM) in soils and its contribution to mineral-associated carbon pool. The underlying mechanisms are identified by estimating its spectroscopic and molecular signatures and comparing its sorption properties on model minerals with natural organic matter (NOM). The results show that MP-DOM leads to 21–576% higher CO 2 emissions and 34–83% lower mineral-associated organic carbon in soils than NOM, depending on the type of plastic polymer. DOM from biodegradable microplastics induces higher CO 2 emissions than conventional microplastics. It is found that MP-DOM is 7.96 times more labile than NOM, making it more accessible for microbial utilization. The lower degree of humification, fewer polar functional groups, and higher H/C ratios in MP-DOM also led to 3.96 times less sorption with mineral particles. The findings provide insights into the effects of microplastics on soil carbon storage and highlight their consequences for wider terrestrial carbon cycling and climate warming.
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JOURNAL OF SURFACTANTS AND DETERGENTS
·
2025
·
IF 1.8
Sihang Ma,Yuanyuan Wang,Qingfeng Hou,Yifeng Liu,Xiaoling Yi,Zhuoyan Zhu,Zhidong Chang
In the petroleum and petrochemical industries, oil sludge is a common contaminant that causes environmental pollution and resource wastage. Currently, recovering crude oil from oily sludge presents a significant challenge during processing. In this study, an amidinium bicarbonate-based CO 2 -responsive microemulsion was developed to effectively treat sludge and recover crude oil. The microemulsion system demonstrates a strong capability for oil solubilization. After the microemulsion treatment, the residual oil contents in the sludge can be reduced to as low as 2.93% (ME-1, n-butanol as cosurfactant) and 1.44% (ME-2, n-hexanol as cosurfactant). Complete oil/water phase separation can be achieved by introducing N 2 at 65°C.
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Materials Today Communications
·
2024
·
IF 3.7
Zhihua Feng,Bo Tang,Kexin Liu,Qingqing Hou,Zhangting Dang,Cui Yang,Xiufu Hua,Qiushuo Yu,Lingling Wang,Renbo Wei
The chemical transformation of CO 2 into high-value-added products is not only favourable to environmental preservation, but also promising for economy. Developing novel and practical catalysts play a critical role in facilitating conversion of CO 2 and the synthesis of high value-added chemicals. Herein, we present the fabrication of biphenyl-typed copper phthalocyanine polymer (BPh-CuPc) from 4,4’-bis(3,4-dicyanophenoxy)biphenyl via a one-pot synthesis procedure, and application of it as a promising catalyst for CO 2 conversion into cyclocarbonate. FTIR, XPS, UV–vis, TGA and SEM measurements confirm the successful fabrication of BPh-CuPc. Attributing to the existence of copper ions which can act as a Lewis acid to activate epoxide, and phthalocyanine rings that is positive for CO 2 absorption, within the chemical framework of BPh-CuPc, it exhibits excellent catalytic activity for CO 2 conversion into cyclic carbonates under mild conditions when combined with tetrabutylammonium iodide (TBAI). As a result, a 98 % yield and 99 % selectivity are obtained for the BPh-CuPc/TBAI system in CO 2 /propylene oxide conversion under condition of 90 °C, 8 h and 2.0 MPa. The obtained high yield and selectivity, as well as remarkable stability and versatility, validate the promising application of BPh-CuPc as a CO 2 conversion catalyst. Synopsis Attributing to the existence of copper ions and phthalocyanine rings within the chemical framework, BPh-CuPc exhibits excellent catalytic activity for CO 2 conversion into cyclic carbonates under mild conditions.
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ACS Applied Polymer Materials
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2024
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IF 4.4
Shangzhong Zhang,Lifeng Yan
Direct conversion of CO2 to polymers, such as polyurea, is an effective approach for CO2 capture and utilization. However, traditional methods involving CO2 and diamine polymerization require high pressures and temperatures (>5 MPa, ∼180 °C) and result in low molecular weight polyurea. A method has been developed to synthesize polyurea directly from CO2 at mild temperature and pressure (0.1–0.5 MPa, 15–90 °C) in a one-step reaction using organic superbases as both catalysts and dehydrants with the formation of DBU-H2O. This process allows for fast polymerization (10–30 min) and yields high molecular weight polyurea (>106 g/mol). The tensile strength of the as-prepared polyurea film reaches 13.5 MPa, which indicates excellent mechanical properties.
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JACS Au
·
2025
·
IF 8.7
Xuan Bie,Yukun Pan,Xiaowei Wang,Shiyu Zhang,Jiahui Hu,Xiaoxiao Yang,Qinghai Li,Yanguo Zhang,Robert E. Przekop,Yayun Zhang,Hui Zhou
Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water–gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N2 and H2.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yingxuan Wen,Fangfang Zhang,Jingru Dou,Shougui Wang,Fei Gao,Falong Shan,Jipeng Dong,Guanghui Chen
The abundant triazine rings with the good affinity for CO 2 molecules in covalent triazine frameworks (CTFs) can capture and activate CO 2 molecules, making CTFs a potential candidate for CO 2 cycloaddition reaction. However, due to the single active site, the realization of high catalytic performance commonly requires the assistance of cocatalysts or harsh reaction conditions. In this study, several novel ionic covalent triazine frameworks (MCTFs, BCTFs and YCTFs) multifunctional heterogeneous catalysts were synthesized for CO 2 cycloaddition reactions. The prepared CTFs catalysts have outstanding pore structure and uniformly distributed active sites (N Lewis basic sites in triazine ring and Cl – nucleophilic sites). The optimal catalyst MCTF-10 has good CO 2 enrichment capacity and high adsorption selectivity. In addition, the catalyst shows an outstanding catalytic performance for the coupling reaction of CO 2 and propylene oxide, with 96 % of yield and 99 % of selectivity for the product under metal-, solvent- and cocatalyst-free parameters (110 °C, initial CO 2 pressure 1 MPa, 4 h). Even under diluted CO 2 concentration (15 % CO 2 , 85 % N 2 ) and mild conditions (80 °C, 0.1 MPa, 24 h), the synthetized CTFs exhibits an outstanding catalytic activity. The excellent catalytic performance, along with the good cycling stability and broad applicability of epoxides, make it a competitive catalyst for catalyzing the CO 2 cycloaddition reaction.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Ashfaq Ahamd,Chaoran Zhang,Yichuan Gu,Qu Jiang,Ziyang Sheng,Ruohan Feng,Sihong Wang,Haoyue Zhang,Qianqing Xu,Zijian Yuan,Fang Song
Ordered mesoporous materials offer significant advantages in reducing energy barriers, tuning intrinsic reaction pathways, and suppressing undesirable side reactions in electrocatalytic CO2 reduction reactions (CO2RR). Here, we present a straightforward method for the direct electrodeposition of ordered mesoporous CO2RR catalysts on a carbon-based porous transport layer, utilizing lyotropic liquid crystals (LLCs) as templates. The versatility of this method was demonstrated with tin-, bismuth-, and indium-based catalysts, all exhibiting pore sizes on the order of several nanometers. These ordered mesoporous catalysts efficiently and selectively drive CO2RR toward the value-added product of formate. They achieve partial current densities that are 3 to 8 times higher than those of disordered mesoporous reference samples, with a faradaic efficiency (FE) of up to 93% at an optimal potential of −0.9 V vs. RHE. In a flow cell configuration, Sn-based catalysts deliver a current density of ∼200 mA cm−2 over 22 hours at a potential of only −0.65 V vs. RHE. Spectroscopic and electrochemical analyses suggest that the high performance can be attributed to the exclusive exposure of active sites for the formate, improved mass transport, and modulated local microenvironments. Our work demonstrates a simple yet effective method for the direct deposition of efficient and selective catalysts onto electrodes. The insights gained from the underlying mechanisms provide valuable guidance for the design of high-performance CO2RR electrocatalysts.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2017
·
IF 1.591
Lei Liu,Cunchuan Zheng,Hongsheng Lu
We reported two simple and novel CO2-responsive surfactant wormlike micellar systems consisting of commercial anionic surfactant sodium oleate (NaOA) and common hydrophobic tertiary amine N,N-dimethylcyclohexylamine (DMCHA), N,N-dimethylbenzylamine (DMBA). The conductivity, pH, and rheological measurements demonstrated the CO2-sensitive flowing behavior and property, which were attributed to the spherical-wormlike micelles transition, verified by cryogenic transmission electron microscopy (Cryo-TEM) and dynamic laser light scattering (DLS) measurements. Moreover, the transition can be easily cycled more than three times without deterioration of viscosity. Combined with the species distribution curve and 1H NMR spectra, a mechanism of the intermolecular electrostatic interaction and hydrophobic effects was proposed.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2017
·
IF 4.421
Xuepeng Wu,Yongping Huang,Sisi Fang,Caili Dai,Hao Li,Zhongliang Xu,Mingwei Zhao
CO 2 -responsive wormlike micelles based on monomer erucic acid 3-(N,N-dimethylamino)propylamide (EADP) with or without sodium salicylate (NaSal) in aqueous solution were studied and compared with “pseudo” gemini system. The “pseudo” gemini system were formed by a mixture of EADP and maleic acid (MA) with molar ratio between 2:1–1:1. Different morphological transformations of microstructures in response to EADP concentrations, additives and CO 2 stimuli were further investigated in these systems, the wormlike micelle or vesicles can be obtained. The mechanism of these transitions were further investigated by rheology, cryo-TEM and DFT calculation, the results showed that the mechanism behind this transition involved reversible reaction of CO 2 with EADP. The mechanism in this research may give further evidence to the self-assembly of CO 2 -responsive surfactants.
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Journal of CO2 Utilization
·
2018
·
IF 5.503
Xianting Cao,Haizhen A. Zhong,Pengfei Zhang,Hui Zheng
A simple chemical fixation of CO 2 at atmospheric pressure to make valuable benzimidazolones derivates via the o -phenylene-diamines carbonylation reaction catalyzed by DBU/S was developed. Different reaction conditions were examined and optimized. A series of benzimidazolones derivatives were synthesized using NMP as solvent at 413K with excellent yields (80–94%). Various substrates were employed and the results suggested the wide application of our method. The quantum mechanics calculations demonstrated that the complexation of DBU with sulfur significantly enhanced the reaction. This protocol rovides a novel approach of fixing CO 2 at atmospheric pressure into a series of 2-benzimidazolones derivates.
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CHEMICAL ENGINEERING SCIENCE
·
2018
·
IF 3.306
Jiamin Hou,Yanying Wei,Sheng Zhou,Yanjie Wang,Haihui Wang
We propose a strategy for rapid in situ fabrication of zeolitic imidazolate framework-8 (ZIF-8) hybrid membrane with assistance of the two dimensional (2D) graphitic carbon nitride (g-C 3 N 4 ) nanosheets at room temperature. The negatively charged g-C 3 N 4 nanosheets with abundant nitrogen coordinating sites are capable to capture and anchor Zn 2+ and thus provide a large number of heterogeneous nucleation sites for the formation of initial ZIF-8 crystals. During the cyclical spin coating of the Zn 2+ /g-C 3 N 4 nanosheets and the ligand (2-methylimidazole), the in situ formed ZIF-8 crystal nucleus on g-C 3 N 4 nanosheets promote the further growth of continues defect-free membranes. The ZIF-8/g-C 3 N 4 membrane with thickness of ∼240 nm can be obtained using this strategy within 30 min at room temperature, which is attractive for fast and facile preparation of molecular sieving membranes. Moreover, it exhibits promising H 2 /CO 2 separation performance with the selectivity up to 42, which is superior to many other ZIF-8 membranes.
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