JOURNAL OF SOLUTION CHEMISTRY
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2020
·Vol. 49
·期 3
·257-271
·
IF 1.273
Zhu Xiao,Song Mengling,Ling Baoping,Wang Sihan,Luo Xiaoyan
Abstract A novel anion-functionalized protic ionic liquid (IL), [DBUH][Triz], has been synthesized from 1,8-diazabicyclo [5.4.0]undec-7-ene (DBU) and 1,2,4-triazole (Triz). Density ( ρ ) and viscosity ( η ) of [DBUH][Triz] at different temperatures have been measured and the influence of temperature has been analyzed quantitatively. Then, the applications of [DBUH][Triz] in CO 2 absorption have been investigated. It has been detected that this ionic liquid, which was easily prepared, shows excellent reversibility and a high absorption capacity, about 1.5 mol CO 2 per 1 mol of IL (about 0.3 g CO 2 per 1 g of IL). In addition, the influence of temperature, pressure and moisture on the absorption performance of [DBUH][Triz] has been studied separately, indicating that absorption is promoted by lower temperature and higher CO 2 pressure. In addition, the mechanism of chemical absorption at two active sites has been deduced based on quantum-chemical calculations and 13 C NMR spectra coupled with IR spectra. Furthermore, the equilibrium constant of chemical absorption ( K ) was calculated from the CO 2 capacity at different temperatures ( T ) and a good linear relationship between the natural logarithm of the equilibrium constant ln K and 1/ T was obtained with R 2 of 0.996. From the slope and intercept of the fitted straight line, the molar reaction enthalpy change (Δ r H m ) and molar reaction entropy change (Δ r S m ) were analyzed, indicating that the capture of CO 2 is an exothermic process and the IL–CO 2 complex is less ordered than the pure ionic liquid. Graphic Abstract
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Scientific Reports
·
2020
·Vol. 10
·期 1
·1-8
·
IF 3.998
Wang Tao,Wang Xinru,Hou Chenglong,Liu Jun
Obstacles to widespread deployments of direct air capture of CO 2 (DAC) lie in high material and energy costs. By grafting quaternary ammonium (QA) functional group to mesoporous polymers with high surface area, a unique DAC adsorbent with moisture swing adsorption (MSA) ability and ultra-high kinetics was developed in this work. Functionalization is designed for efficient delivery of QA group through mesopores to active substitution sites. This achieved ultra-high kinetics adsorbent with half time of 2.9 min under atmospheric environment, is the highest kinetics value reported among DAC adsorbents. A cyclic adsorption capacity of 0.26 mmol g −1 is obtained during MSA process. Through adsorption thermodynamics, it is revealed that adsorbent with uniform cylindrical pore structure has higher functional group efficiency and CO 2 capacity. Pore structure can also tune the MSA ability of adsorbent through capillary condensation of water inside its mesopores. The successful functionalization of mesoporous polymers with superb CO 2 adsorption kinetics opens the door to facilitate DAC adsorbents for large-scale carbon capture deployments.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Jian-Lei Qi,Dan Zhou,Qin-Qin Xu,Jian-Zhong Yin,Kun-Peng Yu,Hai-Xin Sun
In recent years, single-atom catalysts (SAC) have emerged as a new frontier in the field of heterogeneous catalysis owing to their unique properties and minimized metal dosage. Herein, the Pd-ZIF-8 single-atom catalyst was successfully fabricated using ZIF-8 as support, and Pd(hfac) 2 as the precursor using the supercritical CO 2 deposition method. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM) images confirmed the formation of uniformly dispersed Pd atoms. Supercritical CO 2 has the advantage of zero-surface tension and high diffusibility, it can carry the molecules of Pd precursor into the micropores of ZIF-8. The dissolution and diffusion of precursor were observed by a visual view cell and the mechanism of the preparation was analyzed. Finally, semi-hydrogenation of phenylacetylene to styrene was performed to evaluate the catalytic activity of the prepared Pd-ZIF-8 catalyst. The conversion rate of 80.7% and selectivity of 92.2% were obtained at 70 °C and 4 h in the semi-hydrogenation of phenylacetylene.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xiaohong Ma,Danyang Li,Yuheng Jiang,Huacheng Jin,Liuyang Bai,Jian Qi,Feifei You,Fangli Yuan
Utilizing solar energy to convert carbon dioxide (CO 2 ) into chemical fuels could simultaneously mitigate the greenhouse effect and fossil fuel crisis. Herein, a heterogeneous photocatalyst of ZnO nanofiber deposited by Pt nanoparticles was successfully synthesized toward photocatalytic CO 2 reduction via radio-frequency thermal plasma and photo-deposition method. The Pt nanoparticles were introduced on the surface of ZnO nanofibers to broaden the light absorption and utilization, increase the additional reaction active sites and facilitate the separation of photo-generated electron/hole pairs. Combined with the natural advantages of short transfer path of charge carriers and self-support effecting in humid reaction environment for nanofibers, the Pt/ZnO hetero-junction nanocomposites displayed superior photocatalytic activity for CO 2 reduction with respect to bare ZnO nanofibers, affording a CO-production rate as high as 45.76 μmol g −1 h −1 under 300 W Xe lamp irradiation within a gas–solid reaction system. Furthermore, in-suit Fourier transform infrared (FTIR) spectra were applied to unveil the details during photocatalytic CO 2 reduction. This work presents a hetero-junction nanocomposite photocatalyst based on eco-friendly semiconductor and metal materials.
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FOOD HYDROCOLLOIDS
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2022
·
IF 11.504
Hao Zhang,Tuo Zhang,Jiachen Zang,Chenyan Lv,Guanghua Zhao
CO 2 is a greenhouse gas and a major contributor to global warming . Efficient conversion of CO 2 into high value-added food materials represents a promising strategy to decrease CO 2 concentration. In this study, we reported that Ca 2+ -crosslinked alginate beads loaded with carbonic anhydrase (CA) can efficiently catalyze conversion of CO 2 into porous vaterite CaCO 3 particles via a carboxymethyl cellulose (CMC) inducing process. CA encapsulated within the Ca 2+ -crosslinked alginate beads maintained around 100% activity of its original activity after 10 assay cycles. Functionally, the CA-loaded alginate beads facilitated conversion of CO 2 into porous vaterite CaCO 3 particles with high CO 2 removal efficiency in the presence of carboxymethyl cellulose. Notably, such vaterite CaCO 3 particles can be explored for adsorption of astaxanthin with higher loading capacity (2.0 wt %), consequently improving the photo- and thermal-stability of this pigment.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2020
·
IF 7.864
Dewang Zeng,Yu Qiu,Li Ma,Min Li,Dongxu Cui,Shuai Zhang,Rui Xiao
The chemical looping process is promising for CO2 conversion because of the much higher CO2 conversion efficiency than the photocatalytic and electrocatalytic processes. Conventional oxygen carriers have to include a high content of inert support, typically Al2O3, to avoid sintering, thus leading to a trade-off between reactivity and stability. Here, we propose the use of ion-conductive GdxCe2–xO2−δ (GDC) to prepare the supported oxygen carriers. The resulting Fe2O3/GDC materials achieve both high reactivity and stability. Fe2O3/Gd0.3Ce1.7O2−δ shows high CO productivity (∼10.79 mmol·g–1) and CO production rate (∼0.77 mmol·g–1·min–1), which are twofold higher than that of Fe2O3/Al2O3. The performance remains stable even after 30 cycles. The mechanism study confirmed the rate-limiting role of the oxygen-ion conductivity, and the GDC support enhanced the oxygen-ion conductivity of oxygen carriers during the redox reactions, thus leading to improved CO2 splitting performance. A roughly linear relationship between the oxygen-ion conductivity and CO2 yield is also obtained and verified in our testing conditions. This relation can be used to predict and select oxygen carriers with high CO2 splitting performance.
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Journal of CO2 Utilization
·
2024
·
IF 7.2
Yansong Ren,Tianyun Zhang,Shuanjin Wang,Dongmei Han,Sheng Huang,Hui Guo,Min Xiao,Yuezhong Meng
Although triblock polycarbonate thermoplastic elastomers (TPEs) have recently attracted great interests due to their biodegradability, insufficient attentions have been paid to improving the elastomeric properties. Through a tandem reaction strategy involving CO 2 / allyl glycidyl ether (AGE) / cyclohexene oxide (CHO), poly(cyclohexene carbonate)-b-poly(allyl glycidyl ether carbonate)-b-poly(cyclohexene carbonate) (PCAC) is successfully synthesized using a metal-free Lewis acid-base pair catalyst. The synthesized PCACs are pure well-defined ABA triblock all-polycarbonate, which is supported by 1 H NMR, gel permeation chromatography (GPC), and diffusion-ordered spectroscopy (DOSY). A simple modification by grafting alkylthiol chains to PCAC results in excellent TPEs named PCAC-g-S-C a H 2a+1 (PCASaC). The synthesized TPEs are characterized by atomic force microscopy (AFM), thermogravimetric analysis (TG), differential scanning calorimetry (DSC), and mechanical test. They demonstrate a semi-network and semi-domain phase separation structure, wide service temperature range, good strength, high elongation, and extremely high elastic recovery properties. This low-cost, biodegradable, high-performance TPE shows great potential for applications in biomedical, wearable products, sports equipment, and other fields.
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IEEE SENSORS JOURNAL
·
2026
·
IF 4.5
Dingyi Feng,Jing Tian,Changjiang Zhang,Wen Ao,Ying Ma,Fu Liu,Jianlin Zhao,Biqiang Jiang
Reliable and cost-effective detection of percent-level carbon dioxide (CO2) is important for industrial process control, confined-space safety, agricultural storage, and leakage warning, where elevated CO2 levels may pose risks to operational safety and human health. Here, we demonstrate a tilted fiber Bragg grating (TFBG) CO2 sensor integrated with electrospun titanium dioxide/polyimide (TiO2/PI) composite nanofibers. The porous reticular nanofibrous film provides abundant CO2 adsorption sites and continuous gas diffusion channels, while enabling efficient coupling between gases induced material variations and the evanescent field of TFBG cladding modes. CO2 adsorption alters the dielectric properties and effective refractive index of the TiO2/PI coating, thereby perturbing the cladding-mode field and modulating the resonance intensity in the transmission spectrum. After optimization of the TiO2 nanoparticle concentration and electrospun time, the sensor exhibited an intensity sensitivity of 0.050 dB/% within a CO2 concentration range of 0–20%. The enhanced performance arises from the synergy between the CO2 affinity of PI, the active TiO2 sites, the porous nanofibrous coating, and the surface field sensitivity of the TFBG. Benefiting from its simple fabrication process, low material cost, good repeatability, and stable optical response, the proposed TiO2/PI nanofibers integrated TFBG provides a promising optical platform for real-time CO2 monitoring, especially in distributed and low-cost sensing applications.
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INORGANIC CHEMISTRY
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2022
·
IF 5.436
Zhijie Zhang,Liang Li,Ying Jiang,Jiayue Xu
Heterojunction manipulation has been deemed as a promising approach in exploring efficient photocatalysts for CO2 reduction. In this article, a novel step-scheme (S-scheme) photocatalyst of CsPbBr3 quantum dots/BiOBr nanosheets (CPB/BiOBr) was fabricated via a facile self-assembly process. The strong interaction, staggered energy band alignments, and much different Fermi levels between CsPbBr3 and BiOBr promised the formation of an S-scheme heterojunction. The resultant CPB/BiOBr heterojunction delivered remarkable photocatalytic performance in CO2 reduction, with an electron consumption rate of 72.3 μmol g–1 h–1, which was 4.1 and 5.7 times that of single CsPbBr3 and BiOBr, respectively. The superior photocatalytic performance originated from the impactful spatial separation of photoinduced electron–hole pairs, as well as the preservation of strongly reductive electrons for CO2 reduction. This work offers a rational strategy to design S-scheme heterojunctions based on lead halide perovskites, which are expected to have potential applications in the field of photocatalysis and solar energy utilization.
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Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-11
·
IF 4.3
Gao Huimin,Zhang Jinpeng,Zhang Fangyuan,Jing Jieying,Li Wen-Ying
The photocatalytic reduction of CO 2 into formic acid is a feasible approach to alleviate the effects of global climate change and achieve chemical energy storage. It is important to design highly active photocatalysts to improve the selectivity and yield of formic acid. In this study, TiO 2 -based catalysts were prepared and loaded with Pd nanoparticles via an impregnation process. The Pd/H-TiO 2 catalyst demonstrated superior CO 2 reduction activity and a high formic acid production rate of 14.14 mmol cat ·g −1 ·h −1 . The excellent catalytic performance observed in the presence of a Pd/H-TiO 2 catalyst is ascribed to the synergy between O v and Pd. The presence of O v led to increase in CO 2 adsorption while Pd loading enhanced the photogenerated electron-hole pair separation. Electron transfer from H-TiO 2 to Pd also contributed to CO 2 activation.
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JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Songwei Li,Xu Jiang,Hongguang Sun,Shanshan He,Liling Zhang,Lu Shao
Herein, for the first time, mesoporous dendritic fibrous nanosilica (DFNS) is utilized to fabricate mixed matrix membranes (MMMs) to increase the membrane properties and push gas separation performance of low-molecular-weight polyethylene glycol (PEG) impregnated MMMs toward superior CO 2 capture. The basic physicochemical and gas transport properties of various membranes have been examined in detail for clarifying the mechanism of the significant enhancement in membrane performance. The polymer chains around the DFNS became rigidly according to the enhanced T g of the MMMs, gas permeability of the gas improved mainly ascribe to the increase of gas diffusivity . Because of the high porosity of DFNS with the mainly specific pore size range of 2–4 nm, the incorporation of novel mesoporous DFNS in cross-linked CO 2 -philic poly (ethylene oxide) (PEO) matrix can not only promote gas transportation, but also increase the loading rate of low-molecular-weight PEG in membranes. Meanwhile, the introduction of PEGDEM-500 into the DFNS reduces the influence of non-selective interface on the selectivity. We identified the optimized performance of low-molecular-weight PEG impregnated PEO-based MMMs demonstrates the superior CO 2 permeability (up to 2281.1 Barrer, a 478.5% increment than that of original UV cross-linked PEO membrane) and high selectivity (up to 48.1 for CO 2 /N 2 ), which can easily surpass the (2008) Robeson's Upper Bound. The long-term stability of our membrane is also excellent, which makes great promise for CO 2 capture in CCS towards sustainably environmental remediation.
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Frontiers of Environmental Science & Engineering
·
2025
·Vol. 19
·期 6
·1-14
·
IF 6.4
Zhang Tengyu,Zhang Jingxin,Zhang Pengshuai,Tong Yen Wah,He Yiliang,Yang Qing
Anaerobic digestion (AD) is a commonly used technology for facilitating carbon fixation by converting complex organic matter into volatile fatty acids and CH 4 ; however, the issue of CO 2 emission remains unresolved in AD. The formation of amorphous carbon has been identified as a more direct method of carbon fixation in AD. This study aimed to elucidate how amorphous carbon can be formed from organic matter or CO 2 by anaerobic microorganisms. The results showed that amorphous carbon was produced in the anaerobic digestion of inorganic and mixed carbon sources, with yields of 0.38 and 3 µg/10 5 cells, respectively. Its characteristics were analyzed using Raman microscopy. Isotope labeling revealed that CO 2 fixation into amorphous carbon primarily depends on the reversed oxidative tricarboxylic acid cycle (roTCA) and hydroxycaproate. Differential pulse voltammetry combined with gene abundance analysis indicated that flavin electron bifurcation (EB) is involved in electron transfer. The microbial isothermal calorimeter further measured the metabolic calorific value, demonstrating that anaerobic microorganisms can autotrophically fix CO 2 with energy provided by EB. Metagenomic analysis supported the large REDOX equivalents input from EB to sustain the roTCA cycle. This research contributes to understanding the mechanism of CO 2 fixation into solid carbon in anaerobic environments. Additionally, it provides new insights into the potential development of carbon-negative technologies in anaerobic biological treatment.
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