ChemSusChem
·
2024
·
IF 7.5
Dong Li,Kaixuan Wang,Ying Chen,Renyi Li,Jiahong Tang,Yizhou Zhao,Wei Guo,Qi Chen,Yujing Li
Graphical A 0D/1D CPB@TCN heterojunction photocatalyst for CO 2 reduction is synthesized by immobilizing CsPbBr 3 (CPB) quantum dots on one-dimensional porous tubular g-C 3 N 4 (TCN). The strong Pb−N chemical bonding between CPB quantum dots and TCN provides a fast charge transfer channel for the CPB@TCN, which promotes the efficient separation and transfer of photogenerated carriers, resulting in excellent photocatalytic activity. Halide perovskite CsPbBr 3 (CPB) quantum dots (QDs) are considered as a promising candidate for solar-driven CO 2 conversion for their unique optoelectronic properties and suitable band structures. However, the CO 2 conversion efficiency of pristine CsPbBr 3 quantum dots is severely limited due to their rapid electron-hole pair recombination and insufficient active sites. In this study, by immobilizing CPB QDs onto one-dimensional (1D) porous tubular g-C 3 N 4 (TCN), an effective 0D/1D CPB@TCN heterojunction photocatalyst for CO 2 reduction is fabricated. Density functional theory (DFT) calculations combined with experimental studies demonstrate that CPB QDs are uniformly anchored on the surface of TCN through Pb−N chemical bonding, resulting in efficient separation and transfer of photogenerated carriers in CPB@TCN photocatalysts. The resultant CPB@TCN photocatalysts exhibit significantly enhanced photocatalytic activity for CO 2 reduction with the highest conversion rate of 22.62 μmol g −1 h −1 , which is 5.33-times higher than that of pristine CPB QDs. This work unveils the interfacial bonding mechanism of CPB@TCN heterojunction through Pb−N chemical bond, which provides new insights for the development perovskite-based heterojunction photocatalysts.
研究领域:
材料科学
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环境科学
·
化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Juanjuan Yang,Dandan Shao
CO2 to methanol is considered a promising method for CO2 conversion and utilization, yet achieving desirable selectivity remains a significant challenge. Herein, efficient CO2 hydrogenation to methanol is achieved by synthesizing Co0.7ZnO with abundant oxygen vacancies (Ov) through the incorporation of a portion of Co into nanoscale ZnO. By tuning the molar ratio of Co/(Co+Zn) in CoxZnO to increase the Ov content to 71%, CO2 adsorption and activation to form formate (COOH*) are enhanced, thereby reducing the CO selectivity. The efficiency of the hydrogenation of CO2 to methanol was optimized with Co0.7ZnO, which exhibited an impressive methanol formation rate of 2.1 mmol/(g h) and a selectivity of up to 96.7%. The unique structure of incorporating partial Co into nanoscale ZnO to increase the level of Ov not only reduces the level of CO selectivity but also inhibits methane formation, thereby contributing to the high methanol selectivity. This study presents an innovative strategic design through partial doping, which is essential for controlling the selectivity of target products in the CO2 hydrogenation.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SUPERCRITICAL FLUIDS
·
2014
·
IF 2.571
Qin-Qin Xu,Yu-Ling Ma,Gang-Xu,Jian-Zhong Yin,Ai-Qin Wang,Jin-Ji Gao
Well-defined Ag nanowires were obtained in SBA-15 at a short deposition time of 5 min in supercritical CO 2 when adding a small amount of ethylene glycol as the co-solvent. Ethylene glycol played a key role in dictating the nanowire morphology. Through detailed investigation of the whole deposition process, including the dissolution of precursor assisted by the co-solvent, the diffusion properties of the precursor into the nano-scale channels of the substrate, and the interaction between the precursor and the substrate, we found that a small amount of precursors were reduced into Ag 0 by ethylene glycol at the initial stage of the deposition. The resultant Ag 0 then acted as nuclei leading to a non-equilibrium sorption of the precursor. The rapid adsorption of the precursor onto the substrate resulted in a high loading of Ag in a short deposition time and the formation of nanowire morphology. Furthermore, this method was successfully extended to other porous substrates such as γ-Al 2 O 3 , SiO 2 and KIT-6, demonstrating its great potentials in the synthesis of nanocomposites.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Fan Sun,Xueli Xing,Chunyang Zhang,Jinrui Zhang,Hui Hong
Photocatalytic CO2 reduction with naturally abundant H2O as the proton source has attracted widespread concern for its environmental and sustainable advantages. Nevertheless, the high recombination rate of photogenerated electron–hole pairs leads to unsatisfactory solar-to-chemical energy conversion efficiency. In this work, we proposed and validated a strategy that photothermal–magnetic synergistically promotes the separation of photogenerated carriers, as well as their transport, leading to boosted photocatalytic performance. A paramagnetic Z-scheme ZnFe2O4/TiO2 heterojunction was fabricated, and its performance in CO2 reduction was examined under concentrated full-spectrum light illumination with an applied external magnetic field. The built-in electric field of the Z-scheme heterojunction improved the dynamic properties of electron–hole pairs. At the same time, the thermal effect induced by infrared light played a crucial role in promoting CO2 conversion. Importantly, the applied external magnetic field further suppressed the recombination of charge carriers via Lorentz force, magnetoresistance, and spin-polarization effects. As a result, the assistance of a magnetic field significantly increased the yields of CO, CH4, and H2 in comparison to the absence of a magnetic field, with maximum enhancements of 25.3, 29.6, and 62.9%, respectively. Moreover, the excessive heating due to the higher concentrated ratio may induce magnetic disorder within the material, potentially reducing the magnetic field’s ability to facilitate carrier transport. The photothermal–magnetic synergy mechanism was systematically explored. Our work has presented a new approach in which photothermal–magnetic effects synergistically contribute to solar fuel production.
研究领域:
材料科学
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化学工程
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
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IF 5.107
Hao Ling,Sen Liu,Hongxia Gao,Haiyan Zhang,Zhiwu Liang
In order to establish an integrative mass transfer coefficient (K G a V ) model for CO 2 absorption into blended monoethanolamine (MEA)/1-dimethylamino-2-propanol (1DMA2P) solution in packed column, the models of CO 2 Henry’s law constants (He CO₂-MEA/1DMA2P ) and the equilibrium CO 2 solubility (α eq ) were constructed. The experimental produced data can be reasonably analyzed. In this work, the Arrhenius equation was employed to fit the values of He CO₂-MEA/1DMA2P at different temperature with AARD of 4.06%; the Kent-Eisenberg prediction model and empirical polynomial prediction model were used to predict the data of α eq under different CO 2 partial pressures and temperatures with AARDs of 2.64% and 0.83%, respectively; the empirical K G a V model proposed by Li, the empirical K G a V model proposed by Aroonwilas and new K G a V model were used to correlate the average values of K G a V with AARDs of 14.36%, 12.44% and 9.03%, respectively; the model for outlet CO 2 concentration (y CO₂,out ) in packed column was developed with AARD of 15.97%. Moreover, the heat of CO 2 absorption in 6 kmol/m 3 MEA/1DMA2P solution was estimated by Gibbs-Helmholtz equation which gave a value of −39.8 kJ/mol. The results show that the blended MEA/1DMA2P solution has advantages that make it a potential absorbent for CO 2 capture.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
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IF 3.9
Xining Guo,Huiying Li,Leshi Zhang,Rui Hao,Fei Ye,Jianmin Gu,Kaihang Sun,Guozhu Li,Ji−Jun Zou,Zhourong Xiao,Desong Wang
The photothermal catalytic conversion of CO2 into value-added chemicals is of great significance for realizing the goal of carbon neutralization. However, these catalysts have problems such as an insignificant photothermal effect and high recombination of photogenerated carriers. Here, porous TiO2 was prepared by hydrothermal crystallization and topological conversion of metal–organic frameworks (MOFs), and loaded with highly dispersed Pt catalysts to realize an efficient photothermal catalytic reverse water-gas shift (RWGS) reaction. N2-adsorption results showed that the as-prepared Pt/TiO2 catalysts had an abundant mesoporous structure, thus contributing to the rapid diffusion of reactants and light transport. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) results showed that Pt was uniformly dispersed on the catalyst surface with an average particle size of 2.06 nm. H2-TPR profiles showed that the Pt/TiO2 catalyst had strong metal–support interactions, CO2-TPD showed its strong CO2 adsorption capacity, and CO-TPD showed its weak CO adsorption strength. In situ X-ray photoelectron spectroscopy (XPS) showed that the electron cloud density on the Pt surface further increased under light illumination, which contributed to the activation and dissociation of H2. In addition, the Pt/TiO2 catalyst had a narrow band gap width and sufficiently low reduction potential, and its excellent photothermal and photovoltaic properties ensured efficient performance in the photothermal RWGS reaction. The Pt/TiO2 catalysts showed a high CO2 conversion of 29.8%, a product CO selectivity higher than 99.6%, and a stability of more than 3000 min at 350 °C, with a light intensity of 1.2 W cm–2 and a GHSV of 36,000 mL gcat–1 h–1.
研究领域:
催化
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环境化学
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材料科学
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纳米技术
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Changqing Gui,Zirui Wang,Changjian Ling,Zhongfeng Tang
Molten salt-doped MgO adsorbent is considered one of the most promising CO 2 adsorbents in the field. In this work, MgO-based adsorbents were prepared by one-step calcination using MgCl 2 ·6 H 2 O as magnesium source. The CO 2 adsorption performance of MgO-based adsorbents was investigated via different methods. Results showed that the maximum CO 2 adsorption capacity of MgO doped by LiNO 3 -NaNO 3 -KNO 3 was 57.1% at the CO 2 concentration of 80% and 350 ℃, and the MgO-based adsorbents showed good regeneration. The nanosheet structure of the MgO-based adsorbents decreased with the increase in the number of cycles, whereas the crystal structures of MgO and alkali metal nitrates did not change because of multiple decarbonization. DFT computation revealed selective adsorption of CO 2 on different crystal faces of MgO. The (200) crystal face of molten salt-doped MgO did not have CO 2 trap ability. In addition, the doped nitrate did not directly participate in the reaction but reduced the adsorption energy of MgO carbonation. The adsorption energies of the MgO (220) and (222) crystal faces after doping with nitrate were reduced to − 2.07 and − 3.26 eV, respectively. The overall energy level of adsorption decreased as the number of resonance peaks and the stability of the structure increased. This study explains why MgO currently fails to reach the theoretical adsorption capacity and reveals the underlying mechanism of molten salts.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xinyi Wan,Ting Wan,Chaochao Cao,Chengchun Tang,Yanming Xue,Youguo Yan,Zhen Li,Zhizhen Ye,Xinsheng Peng
The development of highly effective and durable CO 2 separation membrane is still a challenge for the carbon capture and storage. Herein, a novel BN nanosheets supported magnetic ionic liquid membrane (BN-SMILM) is constructed by nanoconfining magnetic ionic liquid (MIL) [P 6,6,6,14 ][FeCl 4 ] to the two-dimentional (2D) nanochannels of laminated BN membrane. The 2D nanochannels provide a well support and restricted space for the MIL. The nanoconfinement effect makes the magnetic [FeCl 4 ] - anions align along the center of 2D BN nanochannels, leading to selectively accelerate the CO 2 transport. The nanoconfinement effect and CO 2 separation mechanism are further explicated by the molecular dynamic simulations. As a result, compared with the polymer supported MIL membrane, the as-prepared BN-SMILM exhibits better CO 2 separation performance, with CO 2 permeability of about 227 Barrer and CO 2 /N 2 selectivity of 90 that is above the 2008 Robeson upper-bound. The BN-SMILM also presents excellent long-term stability after 7 days operation, revealing the promising applications in CO 2 separation. This work provides a new strategy to prepare high-performance supported liquid membrane materials towards practical environmental and energy application.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
DOI
高影响因子
Gels
·
2024
·Vol. 10
·期 7
·449
·
IF 5
Huipeng Wang,Changhua Yang,Yongwei Zhang,Chen Wang
In order to solve the problem of gas channeling during CO2flooding in low-permeability reservoirs, a novel CO2responsive gel channeling system was prepared by using carrageenan, branched polyethylene imide and ethylenediamine under laboratory conditions. Based on the Box–Behnken response surface design method, the optimal synthesis concentration of the system was 0.5 wt% carrageenan, 2.5 wt% branchized polyethylenimide and 6.5 wt% ethylenediamine. The micromorphology of the system before and after response was characterized by scanning electron microscopy. The rheology and dehydration rate were tested under different conditions. The channeling performance and enhanced oil recovery effect of the gel system were simulated by a core displacement experiment. The experimental results show that the internal structure of the system changes from a disordered, smooth and loosely separated lamellae structure to a more uniform, complete and orderly three-dimensional network structure after exposure to CO2. The viscosity of the system was similar to aqueous solution before contact with CO2and showed viscoelastic solid properties after contact with CO2. The experiment employing dehydration rates at different temperatures showed that the internal structure of the gel would change at a high temperature, but the gel system had a certain self-healing ability. The results of the displacement experiment show that the plugging rate of the gel system is stable at 85.32% after CO2contact, and the recovery rate is increased by 17.06%, which provides an important guide for the development of low-permeability reservoirs.
研究领域:
石油工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JACS Au
·
2025
·
IF 8.7
Xuan Bie,Yukun Pan,Xiaowei Wang,Shiyu Zhang,Jiahui Hu,Xiaoxiao Yang,Qinghai Li,Yanguo Zhang,Robert E. Przekop,Yayun Zhang,Hui Zhou
Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water–gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N2 and H2.
研究领域:
化学工程
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催化科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Liu Qinglu,Tang Tang,Tian Ziyu,Ding Shiwen,Wang Linqin,Chen Dexin,Wang Zhiwei,Zheng Wentao,Lee Husileng,Lu Xingyu,Miao Xiaohe,Liu Lin,Sun Licheng
Ion-solvating membranes have been gaining increasing attention as core components of electrochemical energy conversion and storage devices. However, the development of ion-solvating membranes with low ion resistance and high ion selectivity still poses challenges. In order to propose an effective strategy for high-performance ion-solvating membranes, this study conducted a comprehensive investigation on watermelon skin membranes through a combination of experimental research and molecular dynamics simulation. The micropores and continuous hydrogen-bonding networks constructed by the synergistic effect of cellulose fiber and pectin enable the hypodermis of watermelon skin membranes to have a high ion conductivity of 282.3 mS cm −1 (room temperature, saturated with 1 M KOH). The negatively charged groups and hydroxyl groups on the microporous channels increase the formate penetration resistance of watermelon skin membranes in contrast to commercially available membranes, and this is crucial for CO 2 electroreduction. Therefore, the confinement of proton donors and negatively charged groups within three-dimensional microporous polymers gives inspiration for the design of high-performance ion-solvating membranes.
研究领域:
材料科学
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电化学
·
分子动力学模拟
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhixiu Yang,Xiaoxuan Guo,Yong Chen,Lijing Gao,Ruiping Wei,Xiaomei Pan,Guomin Xiao
Despite significant advancements in the investigation of catalyst morphology in electrochemical CO 2 reduction (ECR), achieving precise control over multi-carbon (C 2+ ) products selectivity remains challenging. Thus, a sequence of catalysts with incorporation of CuO onto three-dimensional (3D) spherical CeO 2 were synthesized using a hydrothermal and calcination two-step method. The molar ratios of Cu(NO 3 ) 2 ·H 2 O to Ce(NO 3 ) 3 ·6H 2 O can manipulate morphology and oxygen vacancies (O v ) of Cu x Ce y catalysts, further influencing their product distribution in ECR . Materials characterization and electrochemical testing demonstrate that dual effects of spherical morphology and O v in the Cu x Ce y catalysts can enhance the activity and C 2 H 4 selectivity in ECR . To elaborate further on the topic, the pure CeO 2 exhibits excellent Faradaic efficiency (FE) of CH 4 with the value of 54.3 %. Cu 7 Ce 3 , among all Cu x Ce y catalysts, reaches a maximum value of 37.22 % at −1.2 V vs. RHE, possibly attributed to its highest O v concentration. More significantly, the possible reaction pathway was monitor by ATR-FTIR technique for Cu x Ce y during ECR is: CO 2 → *COOH →*CO → *CHO → *OCCOH → C 2 H 4 . The concept of dual tuning strategy by morphology and O v opens up a wide range of possibilities for the development of effective Cu-based catalysts for ECR.
研究领域:
材料科学
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电化学
✓ 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）