APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
·
IF 8.328
Mengli Li,Lingxia Zhang,Xiangqian Fan,Meiying Wu,Min Wang,Ruolin Cheng,Linlin Zhang,Heliang Yao,Jianlin Shi
We have synthesized a series of LaPO 4 /g-C 3 N 4 core-shell nanowires via an in-situ hydrothermal growth of LaPO 4 nanorods in tubular g-C 3 N 4 and investigated their photocatalytic activity in CO 2 reduction. It was found that in the synthesized core-shell structure, the outer g-C 3 N 4 nano-shells coated on the LaPO 4 nanorod cores resulted in the enhanced light absorption and charge carrier separation/transfer ability, thus improved the room temperature photocatalytic performance of the nanocomposites in CO 2 photocatalytic reduction compared with the g-C 3 N 4 and LaPO 4 individuals. A maximum CO yield of 0.433 μmol has been obtained from CO 2 reduction within 1 h irradiation on 30 mg nanocomposite photocatalyst under the absence of any noble metal. Finally, a possible mechanism, which is featured with LaPO 4 activation due to significantly promoted separation/transfer of photo-generated charge carriers, was proposed. The encouraging performance in CO 2 photoreduction demonstrates that this novel nanocomposite will be a prospective material in environmental protection and energy conversion.
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ELECTROCHIMICA ACTA
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2016
·
IF 4.803
Jibo Liu,Huijie Shi,Xiaofeng Huang,Qi Shen,Guohua Zhao
Photo/electrochemical CO 2 reduction using pyridine was feasible to produce methanol via the formation of pyridiniumformate intermediate. To improve the reduction efficiency, a pyridyl bonded ruthenium (II)-based photosensitizer catalyst (Ru-Py) was designed for photoelectrochemical CO 2 conversion. The photocurrent density on Ru-Py modified electrode in CO 2 saturated solution was 0.103 mA cm −2 higher than that without illumination. The total Faradaic efficiency (f) reached 83.1%, whereas the turnover number (TON) for methanol was 38.4 in aqueous solution after 8 h irradiation. The methanol production was 24.1 μmol which was higher than the published literatures (less than 8 μmol) in similar systems could be attributed to the efficient electron transfer between the photosensitizer and the pyridyl active site covalently linked by C-C bond, as well as the strong and wide absorption up to 610 nm resulted from the large conjugated structure of the ligands. The mechanism investigation revealed that the N atom in pyridyl as catalytic active sites played significant role in CO 2 conversion by forming the pyridiniumformate intermediate which was confirmed by the simulation reaction. Meanwhile, in order to realize the reduction process intuitively, the density functional theory (DFT) was applied to simulate the structure of Ru-Py and the pyridiniumformate intermediates.
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ACS Applied Materials & Interfaces
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2016
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IF 7.145
Haiyang Zhang,Ruili Guo,Jinpeng Hou,Zhong Wei,Xueqin Li
In this study, a carbon nanotubes composite coated with N-isopropylacrylamide hydrogel (NIPAM-CNTs) was synthesized. Mixed-matrix membranes (MMMs) were fabricated by incorporating NIPAM-CNTs composite filler into poly(ether-block-amide) (Pebax MH 1657) matrix for efficient CO2 separation. The as-prepared NIPAM-CNTs composite filler mainly plays two roles: (i) The extraordinary smooth one-dimensional nanochannels of CNTs act as the highways to accelerate CO2 transport through membranes, increasing CO2 permeability; (ii) The NIPAM hydrogel layer coated on the outer walls of CNTs acts as the super water absorbent to increase water content of membranes, appealing both CO2 permeability and CO2/gas selectivity. MMM containing 5 wt % NIPAM-CNTs exhibited the highest CO2 permeability of 567 barrer, CO2/CH4 selectivity of 35, and CO2/N2 selectivity of 70, transcending 2008 Robeson upper bound line. The improved CO2 separation performance of MMMs is mainly attributed to the construction of the efficient CO2 transport pathways by NIPAM-CNTs. Thus, MMMs incorporated with NIPAM-CNTs composite filler can be used as an excellent membrane material for efficient CO2 separation.
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Journal of CO2 Utilization
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2017
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IF 4.292
Zhong Ying,Chaoyong Wu,Chao Zhang,Shan Jiang,Ruhui Shi,Haiyang Cheng,Bin Zhang,Yan Li,Fengyu Zhao
A series of polyureas were synthesized with CO 2 as the carbonyl building block, which consist of a hard segment of CO 2 -based oligourea and a soft segment of soluble polyether diamine. The hard segment was formed from 1,3-bis(3-aminopropyl) tetramethyl disiloxane with CO 2 , and the soft segment was obtained through polyaddition of polyether diamine with an extender agent. The Number-average Molecular Weight (Mn) and Weight-average Molecular Weight (Mw) were estimated by Gel permeation chromatography (GPC). The properties of the synthesized polyureas such as thermo-stability and the tensile strength were examined, and these properties could be adjusted by varying the molecular weight of polyether diamine and oligourea segments. The synthesized polyureas have an amorphous structure and presented satisfied thermo-stability (∼250 °C) and the high tensile strength (22.4 MPa).
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CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Chuanwen Zhao,Yafei Guo,Weiling Li,Changsheng Bu,Xinye Wang,Ping Lu
K 2 CO 3 -modified silica aerogels (K 2 CO 3 /SG) were synthesized by the two-step sol-gel and wet impregnation method using K 2 CO 3 and tetraethoxysilane (TEOS) as starting materials and ethanol as solvent. CO 2 sorption behaviors of the sorbent were tested under ultra-dilute flue gas conditions of 20–60 °C, 1%CO 2 , 2%H 2 O and balanced N 2 with gas hourly space velocity (GHSV) of 4000 h −1 using a modified fixed-bed reactor. Experimental CO 2 uptakes of the sorbent under different temperatures were correlated to several kinetics models to study the kinetics performances. The effects of temperature, K 2 CO 3 loading, GHSV, H 2 O:CO 2 molar ratio and H 2 O pretreatment time on CO 2 sorption capacity and kinetics performances of the sorbent were further demonstrated. It is found that the two-step sol-gel and wet impregnation method could benefit the sorbent improved physical properties, superior surface characteristics and enhanced CO 2 sorption performances. Amongst various kinetics equations, the modified Avrami fractional kinetics model could well describe the CO 2 sorption process over K 2 CO 3 /SG. CO 2 sorption capacity decreases with the increase of temperature. With the increasing K 2 CO 3 loading, GHSV, H 2 O:CO 2 molar ratio and H 2 O pretreatment time, CO 2 sorption capacity increases first and then decreases. CO 2 sorption kinetics increases with the increasing temperature and H 2 O pretreatment time, while it decreases with the increasing K 2 CO 3 loading. CO 2 sorption kinetics keeps rather stable and then increases significantly with the increasing GHSV and H 2 O:CO 2 molar ratio.
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ChemSusChem
·
2016
·Vol. 9
·期 17
·2351-2357
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IF 7.116
Mingguang Pan,Ningning Cao,Wenjun Lin,Xiaoyan Luo,Kaihong Chen,Siying Che,Haoran Li,Congmin Wang
Graphical Dual-tuning method : Through the introduction of a large π-conjugated structure into the anion, a dual-tuning approach to improve CO 2 capture by anion-functionalized ionic liquids (ILs) results in high capacities of up to 0.96 ; and excellent reversibility. Quantum chemical calculations, spectroscopic investigations, and thermogravimetric analysis indicate that the increased capacity is a result of stronger dynamic covalent bonds. The strong chemisorption of CO 2 is always accompanied by a high absorption enthalpy, and traditional methods to reduce the absorption enthalpy lead to decreased CO 2 capacities. Through the introduction of a large π-conjugated structure into the anion, a dual-tuning approach for the improvement of CO 2 capture by anion-functionalized ionic liquids (ILs) resulted in a high capacity of up to 0.96 mol and excellent reversibility. The increased capacity and improved desorption were supported by quantum chemical calculations, spectroscopic investigations, and thermogravimetric analysis. The increased capacity may be a result of the strengthened dynamic covalent bonds in these π-electron-conjugated structures through anion aggregation upon the uptake of CO 2 , and the improved desorption originates from the charge dispersion of interaction sites through the large π-electron delocalization. These results provide important insights into effective strategies for CO 2 capture.
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APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Degong Ding,Wenbo Lu,Ya Xiong,Xinglong Pan,Jianqiang Zhang,Cuicui Ling,Yonggang Du,Qingzhong Xue
In this paper, we presented a simple method to fabricate size-controlled La 2 O 2 CO 3 nanoparticle by annealing La(OH) 3 nanocrystallines in air atmosphere. The microstructures of the samples were analyzed by high resolution transmission electron microscope (HRTEM), X-ray diffraction (XRD) and scanning electron microscope (SEM). TEM images indicate that the La(OH) 3 precursors consists of uniform ellipsoids with width of 9–15 nm and length of 15–30 nm and La 2 O 2 CO 3 are spheroidal particles with size of 12–25 nm. XRD patterns indicate that La(OH) 3 nanocrystallines are hexagonal phase and transform to monoclinic La 2 O 2 CO 3 after annealing. And then, La 2 O 2 CO 3 nanoparticle is printed on an interdigital electrode as a sensing material for CO 2 detection. La 2 O 2 CO 3 sensor exhibits good cycle stability performance and fast response and recovery (53 s and 120 s) over the wide range of 300–5000 ppm CO 2 in air condition. In addition, we also investigate the effect of oxygen concentration in the background atmosphere on CO 2 response of La 2 O 2 CO 3 sensor. The CO 2 sensing mechanisms for La 2 O 2 CO 3 sensor can be attributed to the interaction of CO 2 with oxygen species on La 2 O 2 CO 3 surface including chemisorption, surface reaction and desorption process, which also can be used to explain other metal oxide based CO 2 gas sensor.
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ENERGY & FUELS
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2024
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IF 5.2
Haorui Liu,Xiaoqiong Wang,Shixun Chen,Shuixia Chen
A novel solid amine adsorbent meso-PDVB@HBPE-x was prepared by impregnating and cross-linking the hyperbranched amine polymer (HBP-NH2) in a mesoporous polydivinylbenzene (meso-PDVB) substrate with an open-cell structure. The optimum preparation conditions were investigated in detail, and the CO2 adsorption performance of prepared adsorbents was conducted by a fixed bed dynamic adsorption system. It is suggested that beneficial from the low viscosity, the intramolecular cavity of HBP-NH2, and the open-cell structure of meso-PDVB, the best adsorbent meso-PDVB@HBPE-8, which was slightly cross-linked with ethylene glycol diglycidyl ether (EGDE), exhibited a high CO2 adsorption capacity of 5.64 mmol/g under 25 °C and wet conditions and quick adsorption kinetics (a high Qb/Qe ratio of 0.92). Compared with the low-molecular-weight amine tetraethylene pentaamine, HBP-NH2 processes a higher molecular weight and is easily modified. Through cross-linking with EGDE, the N content and CO2 adsorption capacity of meso-PDVB@HBPE-8 remained stable during 20 absorption (at 25 °C)–desorption (at 90 °C) cycles under wet conditions, showing great regeneration stability. The adsorbents showed great potential in CO2/CH4 separation, achieving a CH4 productivity of 18.86 mmol/g from a 15 mL of CO2/CH4 (20:80, v:v) mixed gas. The strategy of synergistically designing the amine and substrate porous structures demonstrates its advantage in the practical application of CO2 adsorption and separation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Ying Wang,Fei Liu,Mengqin Yao,Jun Ma,Shuo Geng,Jianxin Cao,Xiaodan Wang
Promoting the efficient formation of methanol intermediates during CO 2 hydrogenation to lower olefins plays a decisive role in improving the catalytic performance of a tandem catalyst. In this study, a series of chromium (Cr)-modified gallium–zirconium oxides with the formula GaCrZrO x (y%) were prepared via the sol–gel method. The characterization and experimental results show that the addition of moderate amounts of Cr not only facilitates the formation of more oxygen vacancies on the surface of GaZrO x but also strengthens the adsorption and activation ability of CO 2 and H 2 , thereby promoting the generation of formate and methoxy intermediates. After coupling with SAPO-34 zeolite, the methanol intermediate produced on GaCrZrO x (y%) is rapidly converted into lower olefins. This integration manner oxide and zeolite catalysts is particularly important for catalytic performance because an appropriate affinity between components can induce the formation of methanol intermediates via the kinetic effect, which limits the reverse water–gas shift reaction at high temperature. The GaCrZrO x (3.0 %)/SAPO-34 tandem catalyst synthesized via grinding and mixing at 390 °C and 3 MPa exhibits remarkable stability and catalytic performance, achieving a CO 2 conversion close to 30 %, a lower olefin selectivity of 85.8 %, and a lower olefin yield of 11.7 %.
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Advanced Science
·
2025
·
IF 14.1
Fengyi Zhong,Jianping Sheng,Chenyu Du,Ye He,Fengying Zhang,Yanjuan Sun,Ying Zhou,Fan Dong
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO 2 reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr 3 -CsPb 2 Br 5 polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface. Compared to CsPbBr 3 nanocrystals, the 113–125 PNs exhibit a remarkable 3.6-fold increase in photocatalytic CO 2 reduction activity (173.3 µmol −1 g −1 within 5 h). Furthermore, Kelvin probe force microscopy results reveal an increase in the built-in electric field within this lattice-matched co-atomic interface from 43.5 to 68.7 mV, providing a stronger driving force for charge separation and directional migration. Additionally, ultrafast transient absorption spectroscopy uncovers the additional charge carrier transfer pathways across this lattice-matched co-atomic interface. Thus, this unique co-atomic interface significantly promotes the interfacial electronic coupling and mitigates the charge transfer barrier, thus facilitating efficient charge separation and transfer. These insights underscore the importance of interfacial structure in heterojunction design and comprehending the intricate interplay between interface and carrier dynamics.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Chunyue Zhang,Zhida Li,Baiqin Zhou,Wei Zhang,Lu Lu
The energy consumption of up to 90 % of the total power input in the anodic oxygen evolution reaction (OER) slows down the implementation of electrochemical CO 2 reduction reaction (CO 2 RR) to generate valuable chemicals. Herein, we present an alternative strategy that utilizes methanol oxidation reaction (MOR) to replace OER. The iron single atom anchored on nitrogen-doped carbon support (Fe-N-C) use as the cathode catalyst (CO 2 RR), low-loading platinum supported on the composites of tungsten phosphide and multiwalled carbon nanotube (Pt-WP/MWCNT) use as the anode catalyst (MOR). Our results show that the Fe-N-C exhibits a Faradaic selectivity as high as 94.93 % towards CO 2 RR to CO, and Pt-WP/MWCNT exhibits a peak mass activity of 544.24 mA mg −1 Pt , which is 5.58 times greater than that of Pt C (97.50 mA mg −1 Pt ). The well-established MOR||CO 2 RR reduces the electricity consumption up to 52.4 % compared to conventional OER||CO 2 RR. Moreover, a CO 2 emission analysis shows that this strategy not only saves energy but also achieves carbon neutrality without changing the existing power grid structure. Our findings have crucial implications for advancing CO 2 utilization and lay the foundation for developing more efficient and sustainable technologies to address the rising atmospheric CO 2 levels.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Xie Liangyiqun,Cai Yanming,Jiang Yujing,Shen Meikun,Lam Jason Chun-Ho,Zhu Jun-jie,Zhu Wenlei
Direct converting low concentration CO 2 in industrial exhaust gases to high-value multi-carbon products via renewable-energy-powered electrochemical catalysis provides a sustainable strategy for CO 2 utilization with minimized CO 2 separation and purification capital and energy cost. Nonetheless, the electrocatalytic conversion of dilute CO 2 into value-added chemicals (C 2+ products, e.g., ethylene) is frequently impeded by low CO 2 conversion rate and weak carbon intermediates’ surface adsorption strength. Here, we fabricate a range of Cu catalysts comprising fine-tuned Cu(111)/Cu 2 O(111) interface boundary density crystal structures aimed at optimizing rate-determining step and decreasing the thermodynamic barriers of intermediates’ adsorption. Utilizing interface boundary engineering, we attain a Faradaic efficiency of (51.9 ± 2.8) % and a partial current density of (34.5 ± 6.4) mA·cm −2 for C 2+ products at a dilute CO 2 feed condition (5% CO 2 v/v), comparing to the state-of-art low concentration CO 2 electrolysis. In contrast to the prevailing belief that the CO 2 activation step ( \({{CO}}_{2}+{e}^{-}+\, * \,\to {}^{ * }{CO}_{2}^{-}\) ) governs the reaction rate, we discover that, under dilute CO 2 feed conditions, the rate-determining step shifts to the generation of *COOH ( \({}^{ * } {{CO}}_{2}^{-}+{H}_{2}O\to {}^{ * } {COOH}+{{OH}}^{-}({aq})\) ) at the Cu 0 /Cu 1+ interface boundary, resulting in a better C 2+ production performance.
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