Small
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2023
·Vol. 19
·期 37
·2300841
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IF 13.3
Yuhan Wang,Jin Wang,Meng Zhang,Song Zheng,Jiahui Wu,Tianren Zheng,Guocan Jiang,Zhengquan Li
Perovskite nanocrystals (PNCs) are promising candidates for solar-to-fuel conversions yet exhibit low photocatalytic activities mainly due to serious recombination of photogenerated charge carriers. Constructing heterojunction is regarded as an effective method to promote the separation of charge carriers in PNCs. However, the low interfacial quality and non-directional charge transfer in heterojunction lead to low charge transfer efficiency. Herein, a CsPbBr 3 –CdZnS heterojunction is designed and prepared via an in situ hot-injection method for photocatalytic CO 2 reduction. It is found that the high-quality interface in heterojunction and anisotropic charge transfer of CdZnS nanorods (NRs) enable efficient spatial separation of charge carriers in CsPbBr 3 –CdZnS heterojunction. The CsPbBr 3 –CdZnS heterojunction achieves a higher CO yield (55.8 µmol g −1 h −1 ) than that of the pristine CsPbBr 3 NCs (13.9 µmol g −1 h −1 ). Furthermore, spectroscopic experiments and density functional theory (DFT) simulations further confirm that the suppressed recombination of charge carriers and lowered energy barrier for CO 2 reduction contribute to the improved photocatalytic activity of the CsPbBr 3 –CdZnS heterojunction. This work demonstrates a valid method to construct high-quality heterojunction with directional charge transfer for photocatalytic CO 2 reduction. This study is expected to pave a new avenue to design perovskite–chalcogenide heterojunction.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-9
·
IF 26.6
Wang Yuhan,Ren Yanxiong,Cao Yu,Liang Xu,He Guangwei,Ma Hanze,Dong Hongliang,Fang Xiao,Pan Fusheng,Jiang Zhongyi
For the first time, the hydrogen-bonded organic frameworks (HOFs)-based mixed-matrix membranes were designed for CO2 separation
A size-controllable method for synthesis of HOF-21 nanoparticles was proposed via diethylamine-modulated framework assembly process
The HOF-21 mixed-matrix membranes exhibited outstanding separation performance with PCO2 of ~ 800 Barrer, and SCO2/CH4 of ~ 40, SCO2/N2 of ~ 60, surpassing the 2008 Robosen upper bound.
研究领域:
材料科学
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环境工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yixue Xu,Xiaoli Jin,Teng Ge,Haiquan Xie,Ruixue Sun,Fengyun Su,Xin Li,Liqun Ye
The van der Waals (vdW) heterojunction formed between two-dimensional materials can break the anisotropy of the electron beam and is an effective method to improve the photocatalytic performance. Herein, vdW heterostructure is successfully constructed between layered Bi 3 O 4 Cl and 2D g-C 3 N 4 for photocatalytic CO 2 reduction. The weak vdW interaction enables Bi 3 O 4 Cl/g-C 3 N 4 with desirable moderate bandgap and built-in electronic field, which can efficiently separate the electron-hole pairs. As a result, Bi 3 O 4 Cl/g-C 3 N 4 heterostructures exhibit better photocatalytic CO 2 reduction activity compared with pure Bi 3 O 4 Cl and g-C 3 N 4 . The optimized Bi 3 O 4 Cl/20%g-C 3 N 4 possesses the highest CO 2 conversion efficiency with CO and CH 4 generation rate of 6.6 and 1.9 μmol g −1 h −1 , respectively. This work not only reports an effective reference for vdW heterojunction system based on Bi-based and g-C 3 N 4 semiconductors, but also contributes to engineering vdW heterojunctions for satisfactory solar energy conversion performance.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Mu Liu,Liren Zheng,Xiaolei Bao,Zeyan Wang,Peng Wang,Yuanyuan Liu,Hefeng Cheng,Ying Dai,Baibiao Huang,Zhaoke Zheng
Atomic layer deposition (ALD) technique has been proved to be an efficient method to synthesize or modify catalyst. In this study, Cu was loaded on different TiO 2 substrates, pristine TiO 2 and black TiO 2 (denoted as H-TiO 2 ) to achieve better CO 2 photocatalytic reduction performance. Both TiO 2 @Cu and H-TiO 2 @Cu exhibited dramatic enhancement for CO and CH 4 production. The peculiar phenomenon of TiO 2 outperforming H-TiO 2 after ALD loading was further studied by a series of characterization methods. Even though H-TiO 2 showed superior performance for photocatalytic CO 2 reduction than TiO 2 , pristine TiO 2 loaded with more Cu 0/+ after ALD deposition surpassed the performance of H-TiO 2 @Cu which possessed less amount of Cu 0/+ and more Cu 2+ . Cu 0/+ is proved to be the crucial factor for CO 2 reduction and it is capable of overshadowing the influence of Ti 3+ and V o . These results indicate that not only will ALD technique significantly enhance the CO 2 reduction performance after Cu deposition, but the substrate employed for loading and the chemical state of loaded material will also influence the subsequent catalytic performance. In addition, our result provides additional experiment evidence for justifying the significance of Cu 0/+ in photocatalytic CO 2 reduction reaction.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Materials Today Sustainability
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2022
·
IF 7.244
R. Zeng,G. Jin,D. He,L. Zhang,D. Chen,Y. Zhang,L. Zhu,Y. Mei,W. Wu,Y. Luo
Utilizing propane and CO 2 as coreactants to produce syngas (CO/H 2 ) via dry reforming shows several advantages over direct propane dehydrogenation and traditional methane dry reforming . It is of great importance to establish high-efficiency catalytic systems that can break C–C bonds and activate CO 2 simultaneously. Herein, acidic H 2 O 2 was applied to etch LaCoO 3 . Surprisingly, highly dispersed Co 3 O 4 at the edges of support along with high oxygen vacancies were obtained from acidic H 2 O 2 treatment. Furthermore, the treated LaCoO 3 catalyst facilitated the generated intermediates of formate to convert into the desired products. The results showed that acidic H 2 O 2 treated LaCoO 3 catalyst can reach 18% for propane conversion and 35% for CO 2 conversion at 550 °C, showing high catalytic activity . Consequently, the present work provides some ideas for the synthesis of efficient LaCoO 3 catalysts for dry reforming of propane.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
·
IF 3.764
Yufei Huang,Xiaowen Zhang,Xiao Luo,Hongxia Gao,Zain Ali Saleh Bairq,Paitoon Tontiwachwuthikul,Zhiwu Liang
The huge energy consumption of rich amine solution regeneration severely restricts the large-scale application and promotion of the CO2 capture process by the amine method. In order to reduce the operating energy consumption during the CO2 capture process using amines, especially the energy consumption of absorbent regeneration, zeolite β/SBA-15 (BS) has been synthesized in this work using the hydrothermal method with zeolite beta (β) as the silicon source; β was used to prepare the novel Zr@BS and Fe–Zr@BS catalysts for amine regeneration. Experiments for CO2 stripping were performed at 370.15 K using amine solvent [monoethanolamine (MEA)] with an initial CO2 loading of 0.50 mol CO2/mol amine. Additionally, all the materials were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, N2 adsorption–desorption experiment, ammonia temperature-programmed desorption, and pyridine adsorption infrared spectroscopy. Also, the catalytic CO2 desorption performances of seven different catalysts (β, SBA-15, three BS catalysts, Zr@BS, and Fe–Zr@BS) were investigated and assessed from the aspects of the cyclic capacity, desorption rate, and energy consumption. Experimental results indicated that the Fe–Zr@BS catalysts exhibited superior catalytic behaviors than other catalysts studied in this work, improving the desorption factor of MEA solution by 212% and bringing down the energy heat by 33% compared with 5 M MEA solution without catalysts. Furthermore, the Fe–Zr@BS catalysts show good stability and easy regeneration and do not influence absorption performance of the amine solution. Moreover, the possible catalytic mechanism for amine regeneration was proposed, and the stability of the material in terms of the structure of the material and the regeneration heat duty were also studied.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Wentao Zheng,Jialing Chen,Yujiao Jia,Nengqi Sun,Shiping Wang,Xianku Wu,Xuehua Zhang
A series of 1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU)/N-heterocyclic DESs aqueous solutions were designed and synthesized as CO 2 capture agents. They showed excellent performance in absorption capacity, especially for the low-pressure CO 2 . The CO 2 loads in the absorbents were higher than 1.0 mol/mol when the pressure was just 0.1 bar. Through a combination of 13 C NMR spectra, FT-IR spectra and absorption experiments, a novel absorption mechanism was proposed. It was the shuttling role of the carbamate generated from CO 2 and nitrogen heterocycles, along with the synergistic roles of the DBU and water, that caused the high absorption capacity of the DBU/N-heterocyclic DESs for CO 2 . Meanwhile, the thermodynamic parameters, the activation energy and the regeneration efficiency were all measured to estimate the absorption performance of the DBU/N-heterocyclic DESs aqueous solutions for low-concentration CO 2 .
研究领域:
化学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yan Xin,Binfei Li,Zhaomin Li,Zongyang Li,Bo Wang,Xiaopu Wang,Mengyuan Zhang,Weitao Li
During the CO 2 flooding process in fractured low-permeability oil reservoirs, the injected CO 2 is prone to channeling along fractures due to severe reservoir heterogeneity, resulting in poor development effect. The CO 2 -responsive gel system shows dual advantages in achieving CO 2 capture and plugging gas channeling to enhance oil recovery. This paper constructed a system with good CO 2 sensitivity based on long-chain alkyl amide propyl dimethyl tertiary amine first. Subsequently, the properties of the system before and after the response were evaluated through rheological test, and its microstructure was characterized by Cryo-TEM. The system exhibited good CO 2 responsiveness, transitioning from low-viscosity solution system to high-viscosity CO 2 -responsive gel system upon contact with CO 2 , with its viscosity increasing by nearly five orders of magnitude. The CO 2 -responsive gel demonstrated excellent shear resistance, viscoelasticity and shear self-repairing ability. The change of microstructure further verified the mechanism of molecules self-assembly in the system under the action of CO 2 . Then, a series of core physical simulation experiments were carried out to comprehensively evaluate the effects of different factors on the injection capacity, plugging characteristics, dynamic filtration damage performance and EOR effect of CO 2 -responsive gel. The gel maintained injectability while achieving an exceptional deep plugging effect, and the plugging rate reached 98.77%. It showed good characteristics of low filtration and permeability damage in low permeability reservoirs, effectively ensuring the fracture plugging effect. After the fracture was plugged by gel, the sweep range of CO 2 to the matrix significantly expanded, and the gas flooding recovery increased by 18.19–21.7%. Finally, the matrix-fracture dual-media chip model was used to conduct microfluidic experiment, the oil displacement characteristics in different displacement stages were visually clarified, and the synergistic plugging and oil displacement mechanism between the CO 2 -responsive gel and CO 2 was summarized. The research results can provide important insights for the green and efficient application of CO 2 -responsive gel in fractured low-permeability reservoirs.
研究领域:
石油工程
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化学工程
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Zhikun Liu,Tao Yan,Han Shi,Hui Pan,Peng Kang
Direct electrochemical CO 2 capture and utilization from flue gas offers appealing route to closing the carbon cycle and avoiding the cost for CO 2 purification. Yet, the low CO 2 concentration in flue gas and competing oxygen reduction reaction (ORR) pose severe challenges for this process. Herein, we report 4-aminobutylphosphonic acid ligand layer capped Ag nanoparticles (NH 2 BPA-Ag) for high-efficiency conversion of simulated flue gas (SFG). The amino group in NH 2 BPA is available for CO 2 capture and activation, while phosphonic acid groups inhibit ORR by desorbing *OOH intermediate. NH 2 BPA-Ag achieves 82% CO Faradaic efficiency (FE CO ) in H-cell for SFG reduction and enhances FE CO 2.6 times over pristine Ag nanoparticles. In a membrane electrode assembly electrolyzer, NH 2 BPA-Ag shows 79.6% FE CO and 38.1% full-cell energy efficiency at 48 mA cm -2 for SFG conversion. This study highlights the strategy of tailoring catalytic microenvironments at molecular level for realizing a highly selective performance.
研究领域:
化学
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材料科学
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环境科学
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电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Yongbiao Sun,Hui Li,Haijun Lai,Yan Yu,Meiling Hou,Chao Fu,Zaizhou Wang,Chunxiang Zhang
Natural gas purification before liquefaction necessitates the use of efficient adsorbents with high selective CO 2 adsorption and easy regeneration. Because of its efficiency and ease of operation, the ion exchange is widely employed to adjust zeolites’ CO 2 adsorption. However, few in-depth mechanistic studies have been undertaken on cation substitution regulation of pore structure and gas–solid interaction, as well as their synergistic effects on CO 2 selective adsorption and zeolite regeneration. In this study, we synthesized Li + and K + -modified 13X and examined their material characteristics, thermodynamics, adsorption kinetics, and the adsorption–desorption performance under various desorption methods. The results showed that the variation in pore structure and gas–solid interaction with cation radius is non-monotonic, resulting in 13XLi and 13XK having better CO 2 selective adsorption than 13X. All zeolites are extremely stable after 10 adsorption–desorption cycles in each regeneration setting. 13X outperforms 13XLi and 13XK in CO 2 desorption at 30 °C, owing to its large non-micropore volume and low gas–solid interaction. 13XK has the lowest CO 2 desorption rate at low temperature but the highest at high temperature, owing to the flat micropore distribution and the progressive gas–solid interaction. Approximately 100 % regeneration of 13XK is achieved with CH 4 purging (150 mL/min) at 150 °C, owing to its smallest cumulative pore volume at 0.5 nm. This research could help to develop efficient cation-modified X zeolites for CO 2 deep removal from CH 4 streams prior to liquefaction, as well as advance the in-depth understanding of cation substitution mechanisms.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Liju Bai,Shijian Lu,Qizheng Zhao,Linlin Chen,Yingjie Jiang,Chunxiao Jia,Siming Chen
Non-aqueous biphasic solvents, which combine the advantages of a non-aqueous absorbent and biphasic absorbent, have attracted increasing attention for CO 2 capture because of their great potential to reduce the energy consumption. This study proposed a non-aqueous N -ethylethanolamine (EMEA)/ N , N -diethylethanolamine (DEEA)-based liquid–liquid biphasic absorbent with p -xylene (PX) to replace 45–65 % of DEEA. The biphasic absorbent comprising 30 wt% EMEA + 5 wt% DEEA + 65 wt% PX (30E5D65P) had the best phase-change behaviour. In this absorbent, 98.8 % of the absorbed CO 2 was in the lower phase of the solvent, with a volume percentage of 35.1 %. This absorbent also showed the best CO 2 -desorption performance, with almost double the CO 2 -desorption amount and maximum CO 2 -desorption rate compared with those achieved using the 30 wt% EMEA + 70 wt% DEEA (30E70D) non-aqueous absorbent. The regeneration energy of 30E5D65P was 1.71 GJ∙t −1 CO 2 , which was reduced by 31 % and 55 % compared with that of the non-aqueous 30E70D absorbent and the aqueous 30 wt% monoethanolamine absorbent, respectively. 13 C NMR analysis and quantum chemical calculations showed that carbamate and PX have a better separation effect than that of EMEA and DEEA, owing to the presence of both polarity and hydrogen bonding. PX with low polarity was beneficial for the separation of carbamate. The carbamate interacted with (protonated) EMEA, (protonated) DEEA and carbamic acid through hydrogen bonds, resulting in the appearance of these components in the lower phase. The carbamate had no hydrogen bond self-aggregation, which may be the reason why there was no crystal precipitation.
研究领域:
化学工程
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环境科学
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能源技术
✓ 已验证
DOI
高影响因子
International Journal of Greenhouse Gas Control
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2016
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IF 4.064
Yu Zhang,Bo Zhao,Jiazong Jiang,Yuqun Zhuo,Shujuan Wang
The enhancement of absorption of CO 2 by propylene carbonate in the presence of TiO 2 nanoparticles was investigated. The influences of solids loading and particle size of TiO 2 nanoparticles on the absorption rate were studied experimentally. The results show that the gas absorption rate can be enhanced significantly in the presence of TiO 2 nanoparticles. The CO 2 absorption enhancement factor firstly increases and then decreases with the increases of solids loadings, which proves the existence of optimal solids loading. The particle size is also a main factor, which affects CO 2 absorption enhancement factor. As the particle size increases, the optimal solids loading gradually increases. A three-dimensional instantaneous numerous-particle di-mechanism model based on the shuttle mechanism as well as a micro-convection mechanism was developed. The results calculated by the model are close to the experimental results, which showed the model can predict experimental data very well.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）