Nanoscale
·
2019
·Vol. 12
·期 4
·2507-2514
·
IF 6.97
Yipeng Bao,Jin Wang,Qi Wang,Xiaofeng Cui,Ran Long,Zhengquan Li
Harvesting solar energy to convert carbon dioxide (CO2) into fossil fuels shows great promise to solve the current global problems of energy crisis and climate change. To achieve this goal, it is desirable to develop efficient catalysts with visible light response to cater for the solar spectrum. CdTe QDs are ideal candidates for absorbing visible light, but it is difficult to directly perform CO2 reduction due to the lack of effective catalytic sites. Herein, we report a strategy for the activation of mercaptopropionic acid (MPA)-capped CdTe QDs for visible-light-driven CO2 reduction, in which iron ions (Fe2+) are immobilized onto CdTe QDs using L-cysteine as a bridging ligand (CdTe-b-Fe). This ligand bridging strategy can immobilize Fe2+ ions on the surface of CdTe QDs as catalytic sites, and these catalytic sites can be conveniently adjusted by directly adding different types or numbers of metal ions. In addition to effectively immobilizing catalytic sites, the bridging ligands can also provide a pathway for electron transport between CdTe QDs and the catalytic sites. The CdTe-b-Fe QD system based on the ligand bridging strategy exhibits excellent catalytic properties: the yield of CH4/CO (two products together) is 126 μmol g−1 h−1, and the selectivity for carbon-based products approaches 98%. This work presents a facile strategy for immobilizing catalytic sites on QDs and provides a platform for designing efficient visible-light driven catalysts for CO2 reduction.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Wei-Shi Sun,Ming-Jie Yin,Wen-Hai Zhang,Shuo Li,Naixin Wang,Quan-Fu An
Excessive CO2 emissions arising from fossil energy utilization pose severe threats to the environment, climate, and biological species. To this end, high-efficiency separation membranes have been developed to mitigate emerging challenges. Bisphenol A ethoxylate diacrylate (BPA) and poly(ethylene glycol) methyl ether acrylate (PEGMEA) were UV-cross-linked in the presence of low molecular weight poly(ethylene glycol) dimethyl ether (PEGDME) to prepare high-performance CO2 capture membranes in a green way. During the entire membrane fabrication process, no additional solvent was involved and no waste of membrane materials occurred, resulting in a green process. The such-prepared membrane presents an outstanding CO2 permeability of 4883 Barrer, a new record for poly(ethylene oxide) membranes, with a high CO2/N2 ideal selectivity of 43 due to the cooperative contribution of BPA and PEGDME. The unprecedented separation performance of our manufactured membrane is even higher than that of the 2019 CO2/N2 upper bound. Considering the rapid, cost-effective, and green fabrication process, our membrane potentially offers a dramatic advantage in alleviating the current greenhouse gas issue and shows great promise for practical applications.
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MATERIALS SCIENCE FORUM
·
2020
·
IF 0
Yang Meng,Xin Yun Wu,Yu Xin Yan,Shuai Liu,Tao Wu,Cheng Heng Pang
Amine-modified solid sorbents have attracted extensive interests in post-combustion carbon capture for power plants. Among various amines, polyethyleneiemine (PEI) is likely to be the most effective and promising candidate. However, previous studies have mainly focused on examining various supports to increase PEI loading and then enhance CO2 adsorption capacity. In this study, one rare earth element (Ce) and 6 first-row transition metals (from V to Cu) in the oxidation states impregnated on PEI incorporated γ-Al2O3 were prepared and investigated as potential catalyst/promotor for base-catalyzed reaction. Thermodynamic analysis, including isothermal and quasi-static CO2 adsorption tests, were implemented to evaluate the performances amongst the 7 metal oxides. The results showed that MnO2, CeO2 and Fe2O3 showed a better performance in isothermal CO2 adsorption at 75°C. Upon quasi-static tests, the results also indicates that the peak adsorption temperatures (Tpeak, a) of V2O5 and Cr2O3 shifted to high temperature region, whilst opposite behavior of MnO2 was observed. In preliminary study, density functional theory (DFT) was also adopted to assist the screening of metal oxide in terms of bond length and adsorption energies.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Mantang Chen,Lihua Zhu,Shaogang Liu,Ren Li,Nan Wang,Heqing Tang
Dissolved cobalt ions (Co 2+ ) are an excellent catalyst for activating peroxymonosulfate (PMS) to generate SO 4 − for the degradation of organic pollutants, but fairly high level of Co 2+ is generally required, which may cause secondary pollution due to its toxicity. Herein, we demonstrate a novel strategy for this catalytic oxidation treatment in which the required Co 2+ addition is very small, being much less than the emission limit of 17 μmol L −1 . This new strategy is based on the much enhanced catalytic effect by the addition of small organic acids (SOAs). In a typical case, all the added diclofenac (30 μmol L −1 ) was degraded in 20 min by using 2 μmol L −1 Co 2+ , 0.15 mmol L −1 PMS and 0.5 mmol L −1 acetate with a degradation rate constant of 0.482 min −1 , which was about 10 times higher than that (0.048 min −1 ) of equivalent Co 2+ -PMS system without acetate. The formation of SO 4 − was greatly enhanced by introducing acetate, and this novel system is universal for enhanced degradation of various organic pollutants. Similarly, formate, propionate, and butyrate also exhibited enhancing effects on the catalytic ability of Co 2+ . The enhancement mechanism of SOAs on catalytic activation of PMS by low-level Co 2+ was also proposed.
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ACS Omega
·
2019
·
IF 2.584
Wenting Si,Bin Yang,Qingni Yu,Lecheng Lei,Jingke Zhu
CO2 emission is generally regarded as the major contributor to global climate change, and polyethylenimine (PEI)-based CO2 adsorbents are promising materials for the capture of low concentration CO2. This paper deals with the deactivation kinetics of PEI-based CO2 adsorbents used for the capture of low concentration CO2. EA and TG analyses demonstrated that thermal degradation and O2-induced deactivation of the adsorbents occurred simultaneously under air exposure conditions. It was found by N2 exposure experiments at the temperature of 50–80 °C that the thermal degradation of PEI-based adsorbents followed a first-order reaction model with an activation energy of 80.98 kJ/mol and a pre-exponential factor of 6.055 × 108 (h–1). The parallel reaction model was employed to distinguish the O2-induced deactivation from the thermal degradation of the adsorbents through air exposure experiments within 50–80 °C. The O2-induced deactivation exhibited a second-order reaction with an activation energy of 74.47 kJ/mol and a pre-exponential factor of 6.321 × 106 (%–1·h–1). The results of simulating the overall deactivation of the adsorbents by the parallel reaction kinetic model were well consistent with those of the experiments, proving that the parallel reaction model was feasible for the description of the deactivation of PEI-based adsorbents.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Dan Liang,Yunfeng Hu,Qiang Bao,Jian Zhang,Jiawei Feng,Penglai Sun,Yutong Ma,Hongsheng Zhang
Rho zeolite was successfully synthesized by hydrothermal synthesis adopting 18-crown-6 as template, and the cations (H + , Na + , K + , Cs + , Cd 2+ and Pb 2+ ) of different radii were introduced into the framework of Rho by ion exchange. The samples were characterized by XRD, SEM-EDX, ICP and N 2 -BET. The adsorption behavior of CO 2 and CH 4 on cation-exchanged Rho was measured, and the adsorption isotherm was fitted by Langmuir equation to study the adsorption performance of these zeolites. The adsorption results show that the pore size of Rho is not solely dependent on the cation radius, the different positions of the cations are also more crucial in pore size adjustment. In all researched Rho, the introduction of Cd 2+ and Pb 2+ can more significantly reduce the pore size, and completely restrict the entry of CH 4 , thereby further improving the CO 2 /CH 4 selectivity. Therein, Cd-Rho has the best adsorption performance, with considerable CO 2 adsorption capacity, and extremely high CO 2 /CH 4 selectivity and CO 2 working capacity, which provides a new clue for the development of adsorbents for CO 2 and CH 4 separation in PSA process.
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CHINESE JOURNAL OF CHEMISTRY
·
2017
·Vol. 36
·期 2
·147-152
·
IF 1.852
Qing-Wen Song,Ping Liu,Li-Hua Han,Kan Zhang,Liang-Nian He
One-pot two-step stepwise reaction of terminal propargylic alcohols, carbon dioxide, and primary/secondary amines for the effective synthesis of various urethanes through robust silver-catalysed C-O/C-N bond formation is reported. Catalytic activities were investigated by controlling catalyst loading, reaction pressure and time, and very high turnover number (turnover frequency) was obtained: 3350 (35 h −1 ) with 0.01 mol% silver catalyst under 0.1 MPa, and up to 13360 (139 h −1 ) with 0.005 mol% silver catalyst under 2.0 MPa at room temperature. The strategy was ingeniously regulated, and synchronously afforded a wide range of β-oxopropylcarbamate and 1,3-oxazolidin-2-one motifs in excellent yields and selectivity together with unprecedented high turnover number (TON) and turnover frequency (TOF) value.
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RSC Advances
·
2013
·Vol. 3
·期 11
·3726-3732
·
IF 2.562
Tian-Yuan Shi,Jin-Quan Wang,Jian Sun,Ming-Hui Wang,Wei-Guo Cheng,Suo-Jiang Zhang
A series of hydroxyl-functionalized poly(ionic liquids) (PILs) were synthesized and employed as catalysts for the synthesis of cyclic carbonates from CO2 and epoxides without the use of any co-catalyst or organic solvent. It was demonstrated that hydroxyl and bromide anion had an excellent synergetic effect on promoting the reaction, and the PILs catalysed co-polymerization of 1-vinyl-3-carboxyethylimidazolium bromide with the cross-linker divinylbenzene (DVB) was observed to be the most efficient, with nearly a 99% yield of propylene carbonate and 100% selectivity. The effects of temperature, pressure and reaction time on the reaction were also investigated. Moreover, the catalysts can be easily recovered and reused more than five times with only a slight decline in catalytic activity. This process carries huge industrial applications due to the reactions high efficiency and the ease of catalyst separation and recycling, which could be profitably applied to the development of fixed-bed continuous flow reactors.
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JOURNAL OF MEMBRANE SCIENCE
·
2014
·
IF 4.908
Xueqin Li,Meidi Wang,Shaofei Wang,Yifan Li,Zhongyi Jiang,Ruili Guo,Hong Wu,XingZhong Cao,Jing Yang,Baoyi Wang
Composite membranes were fabricated by incorporating poly(N-isopropylacrylamide) nanohydrogels (NHs) into Matrimid ® 5218 matrix to improve the separation performance for CO 2 /CH 4 and CO 2 /N 2 mixtures. The membranes were characterized by a fourier transform infrared spectrometer (FT-IR), scanning electron microscopy (SEM), tensile test, dynamic mechanical analysis (DMA), X-ray diffraction (XRD), positron annihilation lifetime spectroscopy (PALS), the static contact angle and water content measurement. The incorporation of nanohydrogels increased the fractional free volume of the composite membranes, water uptake and water retention capacity. The composite membranes displayed better performance than the pure Matrimid ® membrane. The nanohydrogels homogeneously embedded in the Matrimid ® matrix acted as water reservoirs to not only provide more water for dissolving CO 2 , but also construct interconnected CO 2 transport passageways. The as-prepared Matrimid ® /NHs-20 composite membrane showed CO 2 /CH 4 and CO 2 /N 2 selectivities of 61 and 52 with a CO 2 permeability of 278 Barrer, surpassing or being close to the 2008 Robeson upper bound lines.
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Greenhouse Gases-Science and Technology
·
2025
·
IF 2.8
Ziyong Li,Qingdan Huang,Tingyan Wang,Huihong Huang,Haoyong Song
The amino groups and its substituents of organic amine absorbents have an important influence on the CO 2 absorption and desorption performance. In this study, four diamines with the same primary amino group and another different amino groups were selected as absorbents, including 1,3-propanediamine (1,3-PDA), 3-methylaminopropylamine (MAPA), 3-dimethylaminopropylamine (DMAPA), and 3-diethylaminopropylamine (DEAPA). The phase-change absorption system uses a mixture of polyether and H 2 O as the solvent. The CO 2 absorption performance of flue gas was studied with the analysis on absorption and desorption rate, cycle capacity, and desorption ratio. The effect of diamine molecular structures on phase-change CO 2 capture was investigated by nuclear magnetic carbon spectroscopy. The results show that DEAPA exhibits highest absorption capacity of 1.21 mol CO 2 /mol amine and recycling capacity of 1.09 mol CO 2 /mol amine. The absorption rate of primary and secondary diamines in the phase-change system is significantly higher than that of primary and tertiary diamines. The diamine system with tertiary amino groups has significantly faster desorption rate, higher desorption ratio, and cycle capacity than the primary and secondary diamine systems. The intramolecular tertiary amino group is more conducive to promoting the absorption of CO 2 than the intermolecular tertiary amino group, which can increase the absorption rate of CO 2 by the primary amino group and enhance the CO 2 desorption.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yizheng Tao,Lei Wang,Benxing Li,Jin Huang,Yichang Pan
Interfacial compatibility is a critical prerequisite for maximizing the gas separation pot entail of metal-organic framework (MOF)-based mixed-matrix membranes (MMMs). In this study, an innovative strategy that employs polymers of intrinsic microporosity (PIMs) covalently grafted onto MOF surfaces has been introduced to engineer compatible interfaces through graded interfacial bonding. Through the reaction between PIM-COCl functionalized polymers and ZIF-NH 2 nanoparticles at ambient temperature, amide-bonded PZIF-CONH nanohybrids have been synthesized, which exhibited superior dispersibility in both solvent media and polymer matrices. Notably, the PZIF-CONH nanohybrids retained their intrinsic high porosity without encountering the pore-blocking issues commonly associated with conventional surface modifiers, owing to the microporous nature of PIM materials. The PIM-based surface modification establishes strong interfacial interactions between ZIF-particles and the polyimide matrix, leading to the fabrication of defect-free MMMs. These gas separation membranes have demonstrated significantly enhanced CO 2 permeability and CO 2 /CH 4 selectivity, exceeding the 2008 upper bound. The gas-permeable polymeric modification approach can offer a promising solution for enhancing the stability and separation performance of MMMs.
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iScience
·
2025
·
IF 4.1
Kai Chen,Jia−Yi Du,Haoran Zhang,Yingqi Fan,Dong−Yue Yang,Jin Wang,Kai Li,Gang Huang
Lithium (Li)−CO 2 batteries, capable of converting CO 2 to Li 2 CO 3 /C while delivering significant energy, have attracted extensive research interest. However, their feasibility remains controversial and underexplored. To address this, a rigorous testing system combining ECC−Air battery models and differential electrochemical mass spectrometry (DEMS) was developed to ensure a pure gas environment. Findings reveal that even minute O 2 permeation (0.5%) from air can elevate the discharge plateau, misleadingly transforming Li−CO 2 into Li−O 2 /CO 2 batteries. Under strict testing, true Li−CO 2 battery performance falls short of reported successes. Experimental and theoretical confirmation shows the 4Li + 3CO 2 → 2Li 2 CO 3 + C reaction proceeds at a lower discharge plateau (<2.0 V), a voltage window traditionally overlooked. This work underscores the need for rigorous testing to enhance scientific reliability in Li−CO 2 battery research so that this field can develop sustainably.
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