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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DOI
PubMed
高影响因子
NEW CARBON MATERIALS
·
2022
·
IF 3.7
Hong-zhi Wang,Yue-zhu Zhao,Zhong-xue Yang,Xin-ze Bi,Zhao-liang Wang,Ming-bo Wu
Using CO 2 as a renewable carbon source for the production of high-value-added fuels and chemicals has recently received global attention. The photoelectrocatalytic (PEC) CO 2 reduction reaction (CO 2 RR) is one of the most realistic and attractive ways of achieving this, and can be realized effectively under sunlight illumination at a low overpotential. Oxygen-incorporated carbon nitride porous nanosheets (CNs) were synthesized from urea or melamine by annealing in nitrogen or N 2 /O 2 gas mixtures. They were used as the photoanode with Bi 2 CuO 4 as the photocathode to realize PEC CO 2 reduction to the formate. The electrical conductivity and the photoelectric response of the CNs were modified by changing the oxygen source. Oxygen in CNs obtained from an oxygen-containing precursor improved the conductivity because of its greater electronegativity, whereas oxygen in CNs obtained from the calcination atmosphere had a lower photoelectric response due to a down shift of the energy band structure. The CN prepared by annealing urea, which served as the source of oxygen and nitrogen, at 550 °C for 2 h in nitrogen is the best. It has a photocurrent density of 587 μA cm −2 and an activity of PEC CO 2 reduction to the formate of 273.56 μmol cm −2 h −1 , which is nearly 19 times higher than a conventional sample. The CN sample shows excellent stability with the photocurrent remaining constant for 24 h. This work provides a new way to achieve efficient catalysts for PEC CO 2 reduction to the formate, which may be expanded to different PEC reactions using different cathode catalysts.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Miao Zhang,Ruijin Zheng,Ying Ma,Ruiping Chen,Xun Sun,Xuan Sun
Three 2D N-rich COFs linked by –C=N– bond, named COF-SDU1, COF-SDU2, COF-SDU3, have been synthesized via the Schiff-base condensation reaction . Tri-(4-formacylphenoxy)-1,3,5-triazine (TRIF) is employed as N-rich aldehyde building block, and p-phenylenediamine (PA), hydrazine hydrate, and terephthalic dihydrazide (TPDH) are as the amine building blocks, respectively, which results in high crystallinity, high BET surface area, and abundant N-atom sites for COF-SDU1, COF-SDU2, and COF-SDU3. COF-SDU1 exhibits large CO 2 uptake of 741 mg g −1 at 298 K under 45 bar, while COF-SDU2 is 484 mg g −1 and COF-SDU3 is only 331 mg g −1 , which are closely related to their specific surface area but irrespective of the absolute N-content. The result clearly reveals the impact of various factors, including N-content, BET surface area and pore size on CO 2 storage performance. It shows that N-content determines capacities at low pressure (<1 bar), BET surface area plays the decisive role under relative low pressure (<25 bar) and large pore size helps enhance the capacity under relative high pressure (>25 bar). Among all factors, BET surface area plays the crucial role in determining the high-pressure CO 2 storage capacity, which is well verified by theoretical modeling.
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高影响因子
FUEL
·
2022
·
IF 8.035
Weiping Liao,Haoyi Lin,Mengdie Yin,Jiaxing Zhang,Zhiguo Zhu,Hongying Lü
The confinement of metal-based matrix such as clusters, particles and even isolated single atoms in zeolite framework was intensively reported, while it was highly untoward to realize this goal for non-metallic ions due to the mutually-exclusive electrostatic interaction between the zeolite framework with negative charges and non-metallic anions. Herein, confinement of iodide ions in Mg-Beta zeolites (I@Mg-Beta) was successfully accomplished via the methodology of structural reconstruction, whose physicochemical property, channel connectivity as well as the location of Mg 2+ and I - ions were investigated systematically. It was found that Mg 2+ ions were located in the zeolitic framework and I - ions were mainly confined in Mg-Beta zeolite via the electrostatic interaction with tetraethylammonium cations. The establishment of structure–function relationship in CO 2 cycloaddition reaction with epoxides indicated the presence of synergistic effect between framework Mg 2+ ions and confined I - ions. The immobilisation of halide ions onto a zeolite support enabled it the recoverable ability from reaction systems, giving rise to relatively stable reusability. The catalytic transformation of CO 2 cycloaddition with epoxides in this work was devoted to ameliorate environmental stress from anthropogenic greenhouse gases of CO 2 by means of elaborately constructing metallosilicate zeolite confined non-metallic catalysts with dual functions.
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EUROPEAN POLYMER JOURNAL
·
2020
·
IF 3.862
Xiaoyun Li,Junwei Wang,Maoqing Kang,Yuhua Zhao,Qifeng Li,Chen Liang
Carbon dioxide based amino-alcohol compound (CO 2 -AA) with both alcohol and amino units in the molecular was prepared by chemical fixation of CO 2 with 1, 4-butanediol diglycidyl ether and ethylenediamine, which was further used as chain extender to the preparation of waterborne polyurethanes (CO 2 -WPUs). Since the reacting activity of isocyanate groups in WPU prepolymer with NH 2 was much faster than that with OH, hydroxyl groups could be maintained in the system and strengthen the hydrogen bonding interaction in WPU endowing the materials with some special properties. Specifically, the unique structure of CO 2 -AA improved mechanical, water/solvents resistance and hydrolysis/oxidation resistance properties of CO 2 -WPUs. Mechanical properties of the CO 2 -WPUs changed slightly during immersion in water, 0.25% NaOH and 6.00% H 2 O 2 solution, while the WPUs prepared from typical chain extender ethylenediamine almost lost their mechanical properties after immersed in the solutions for 5 h. Moreover, the CO 2 -WPU films showed considerable thermal stability. The study suggested the novel CO 2 -AA might be a promising chain extender to improve the water/solvent resistance and hydrolysis/oxidation resistance of WPU.
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高影响因子
FUEL
·
2016
·
IF 3.611
Yingchao Hu,Wenqiang Liu,Hongqiang Chen,Zijian Zhou,Wenyu Wang,Jian Sun,Xinwei Yang,Xian Li,Minghou Xu
A screening of inert solid supports as metal skeletons of CaO-based sorbents was conducted in this work, aiming to provide the basis and guideline for the selection of inert solid refractories to produce high temperature CO 2 capture sorbent. We studied 12 different refractories including Al-, Ti-, Mn-, Mg-, Y-, Si-, La-, Zr-, Ce-, Nd-, Pr- and Yb-based supports, among which Yb and Pr are newly introduced ones. The sorbents were synthesized using the same wet-mixing method, by which the inert supports could be well dispersed among the ultra-fine active specie of CaO/CaCO 3 particles to fully play the role of frameworks for sintering resistance. The sorbents stabilized by these inert supports were also cyclically tested under the same conditions. Y- and Al-based supports were found to exhibit much superior cyclic performance than the other supports. Mn-, Mg-, La-, Yb- and Nd-based supports are also good candidates, whereas the other ones containing Ti-, Ce-, Zr-, Si- and Pr-based supports show less effectiveness. The melting point of the inert support and surface area of the synthetic sorbents are found to be the key factors to affect the sorbent performance.
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高影响因子
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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高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Beibei Zhang,Lihua Zhang,Jin Li,Jiawen Fu,Xiwei Qu
In the present work, a series of PVA and CS blend membranes were studied. These prepared membranes were evaluated by binary mixture gases of CO 2 /N 2 and CO 2 /CH 4 . The optimum ratio of PVA/CS for CO 2 permeance was achieved at 5:5. It recorded a CO 2 permeability of 20.8 GPU (1 GPU = 1 × 10 -6 ·cm 3 (STP)·cm −2 ·s −1 ·cmHg −1 ) with CO 2 /N 2 selectivity of 89.7, as well as CO 2 permeability of 10.2 GPU and CO 2 /CH 4 selectivity of 56.3. Secondly, two kinds of nanoparticle UiO-66 and UiO-66-NH 2 were used to prepare mixed matrix membranes. The effects of nanofiller content and chemical groups on gas permselectivity were investigated. Results show that the addition of nanoparticles can effectively improve the permselectivity of membrane. The mixed matrix membranes addition with UiO-66-NH 2 achieved the optimum CO 2 performance and these were following the order of PVA(5)/CS(5)-UiO-66-NH 2 > PVA(5)/CS(5)-UiO-66 > PVA(5)/CS(5). For all these membranes, the permeance and selectivity present initial increased and then decreased. Mixed matrix membranes addition UiO-66-NH 2 (containing 3.75 wt%) exhibits a CO 2 permeance of 32.77 GPU and CO 2 /N 2 selectivity of 93.47, as well as CO 2 permeance of 25.57 GPU and CO 2 /CH 4 selectivity of 70.1, which was beyond the 2008 Robeson upper bound.
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高影响因子
OPTICS EXPRESS
·
2019
·Vol. 27
·期 3
·1991-2000
·
IF 3.561
Hanyang Li,Bo Sun,Yonggui Yuan,Jun Yang
A carbon dioxide (CO2) gas sensor based on a polyhexamethylene biguanide (PHMB)-coated whispering gallery mode (WGM) microbubble resonator is proposed and verified experimentally in this work. Microbubbles were fabricated using two reverse arc discharges focused on microcapillaries. The inner wall of the microbubble was coated with a layer of PHMB using a filling and sintering process. A significant WGM resonance was observed by coupling with a tapered fiber. The experimental results show that as the concentration of carbon dioxide increases, a blue shift appears in the spectrum. Addition, a high sensitivity (0.46 pm /ppm) and a good linear relationship were obtained in the measurement range of 200-700 ppm with a detection limit of 50 ppm. The sensor features include high sensitivity, simple structure, easy manufacture, and low cost.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2016
·
IF 2.628
Li Liu,Na Tian,Long Huang,Yu-Hao Hong,Ai-Yun Xie,Feng-Yang Zhang,Chi Xiao,Zhi-You Zhou,Shi-Gang Sun
The modification of oxide-derived Cu electrode with Ni, Zn, and Au was examined to improve the catalytic activity of CO 2 electroreduction. The experimental results showed that Ni modification increased the Faraday efficiency of the formation of formic acid and n -propanol. The Faraday efficiency relating to the formation of the liquid products was as high as 34.3% at −1.5 V versus the saturated calomel electrode reference potential. In contrast, modification with Zn reduced the formic acid formation efficiency but enhanced the alcohol formation efficiency. Finally, modification with Au suppressed the selectivity toward the formation of both formic acid and alcohols.
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DOI
高影响因子
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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高影响因子
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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DOI
PubMed
高影响因子
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