APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Liang Fu,Zhenping Qu,Lingling Zhou,Yue Ding
Interface engineering is demonstrated to lead to significant improvement in the catalytic performance for electrochemical CO 2 reduction reactions (CO 2 RR). In this work, we demonstrate a heterogeneous In(OH) 3 -Ag interface catalyst in which the appropriate In(OH) 3 clusters modified on metal Ag nanoparticles surface greatly improves the CO selectivity in CO 2 RR, realizing a CO faradaic efficiency (FE CO ) of 93% at − 0.7 V vs. RHE. The performance enhancement is attributed to the preferentially CO 2 adsorption and activation by the In(OH) 3 -Ag interface sites. In situ Raman spectroscopy reveals that the formation of In(OH) 3 -Ag interface sites is significantly favorable for the generation of key *CO 2 − intermediate at low overpotential. Further theoretical calculation confirms that the In(OH) 3 -Ag interface could enhance the adsorption of *COOH species on catalyst by means of tailoring the surface properties and electronic structures. This work shows that hydroxide-metal interface engineering is a promising pathway to regulate the activity for selective CO 2 RR properties.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Progress in Natural Science-Materials International
·
2024
·
IF 4.8
Shijia Liu,Haibin Wang,Xi Wang,Jieshu Zhou,Hongyan Liang
Electroreduction of CO 2 for formic acid production has been regarded as an efficient option for CO 2 utilization. However, under high current, achieving high selectivity for formic acid is challenging, which cannot meet industrial demands. Herein, we reported a type of Bi/In(OH) 3 (BIO) heterojunction reconstructed from Bi 2 S 3 /In(OH) 3 during electrochemical process, in which In(OH) 3 was applied to modulate the electronic structure of Bi. This strategy efficiently enhanced the ∗OCHO intermediates adsorption and lead to a decent selectivity towards formic acid under high current density. BIO displays faraday efficiency of formic acid beyond 95 % across a wide range current density of 200–400 mA cm −2 , where the highest value reached 97.7 % at 400 mA cm −2 . This work clarified the mechanism of CO 2 electroreduction to HCOOH on heterojunction, guiding the design of advanced catalysts.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jingyun Qian,Wenna Zhang,Xue Yang,Kexin Yan,Meikun Shen,Hongyue Pan,Hongjun Zhu,Lei Wang
Constructing the metal cation-mediated low-cost inorganic sorbent with high separation efficiency in CO 2 , N 2 , and CH 4 remains a major challenge. Herein, we developed a series of alkali metal cations (Na + , K + , Rb + , Cs + )-exchanged ERI zeolites and adopted in the separation process of CO 2 among the gas mixture. Among the ion-exchanged zeolites, the zeolite K-ERI showed a high adsorption volume of 70.84 cm 3 g −1 and an IAST selectivity of CO 2 /CH 4 : 6254, CO 2 /N 2 : 2872 at 298 K, respectively, far outweighed the reported metal cation exchanged zeolites. Combining powder X-ray diffraction crystallography and density functional theory calculations, we unequivocally unveiled that the metal cations located at s 8 r effectively tailored zeolite aperture, and metal cation-gas molecules interactions synergically restrained the pass-through capacity of CO 2 in ion-exchanged ERI framework. Such a unique host–guest interaction governed by metal cations in aluminosilicate zeolite ERI affords a general strategy for gas separation.
研究领域:
材料科学
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化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Shu Panxiang Chen,Xiaoyu Sun,Xiao Luo,Zhiwu Liang
In this study, Li/Al hydrotalcite (HT) was treated with calcination and potassium hydroxyl-ethanol to form bcHT (basic-modified calcined hydrotalcite). This material was then polyethylenimine (PEI)-functionalized to create a new sorbent that has ultralow energy consumption. Various methods were applied to characterize the sorbent, including N2 adsorption–desorption, Fourier transform infrared spectroscopy, X-ray diffraction, and scanning electron microscopy. CO2 adsorption capacity, which was affected by PEI loadings and adsorption temperatures, was assessed with the CO2 adsorption isotherms and cyclic CO2 adsorption–desorption performance. Results showed that the optimal CO2 adsorption capacity of 1.723 mmol/g was reached when operating with temperature of 323 K and PEI loading of 40%. The Freundlich model was applied to provide optimal correlations with the experimental data, and the correlation coefficients reached 0.997. The average isosteric heat of CO2 adsorption was calculated to be 67.492 kJ/mol. The relatively low desorption energy consumption was calculated to be 63.20 kJ/mol with the Amenomiya equation. Four kinetic models were applied to analyze the kinetics of PEI-functionalized bcHT, and both the Avrami’s fractional order model and DEM model were well fitted to the experimental data. The activation energy of the bcHT-PEI-40% was 30.34 kJ/mol calculated by the Avrami’s fractional order model, which is obviously lower than the values of the CO2 adsorption with traditional amine solution.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Zhenkang Li,Zhiping Wang,Qiwei Yang,Zhiguo Zhang,Yiwen Yang,Qilong Ren,Huabin Xing
Ionic liquid (IL)-mediated extraction methods have drawn much attention due to their reduced environmental impact and improved extraction efficiencies compared to traditional separation methods. However, one long-standing challenge in the application of IL-based extraction processes is the difficulty in recovering high-boiling solutes from the IL phase due to the negligible vapor pressure of ILs and the strong interaction between solutes and ILs. In this study, a new CO2-assisted back-extraction method was developed for the recovery of high-boiling solutes from the IL phase based on the reversible chemical absorption and/or strong physical interaction of CO2 with ILs. We found the distribution coefficient (D) of the typical solute δ-tocopherol in the [P4444][Pro]/DMSO–hexane biphasic system significantly decreased from 10.38 to 2.42 after the introduction of CO2, which greatly reduced the required solvent consumption and the number of back-extractions required for tocopherol recovery. For example, the number of back-extractions required for the recovery of 90% of the tocopherols from the [P4444][Pro]/DMSO–hexane biphasic phase decreased from 24 to 5 with the aid of CO2 absorption, along with a decrease in solvent consumption by approximately 80%. The effects of the structure of the IL, the loading of CO2, the type of cosolvents, and the temperature of the CO2-assisted back-extraction processes were investigated in this study. This proof-of-concept study demonstrates the great potential of CO2-assisted back-extraction as a green method for the efficient recovery of high-boiling solutes from the IL phase.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2025
·
IF 7.7
Jinxu Hao,Xianda Sun,Baibin Ma,Wanzhen Huang,Yuandong Yang,Xiaohan Ren
The carbon-neutral and carbon-negative energy utilization technologies have long been people pursued to realize the strategic objective of carbon neutrality. Herein, we propose a cation-exchange membrane (CEM) direct formate-CO 2 fuel cell that possesses the capability of simultaneously generating electricity and producing hydrogen, as well as continuously transforming carbon dioxide into pure sodium bicarbonate. Using the CO 2 -derived formate fuel, the roof-of-concept CEM direct formate-CO 2 fuel cell exhibits a peak power density of 38 mW cm −2 at 80 °C without the assistance of additional electrolyte. The fairly stable constant-current discharge curve along with the detected hydrogen and pure sodium bicarbonate prove the conceptual feasibility of this electricity‑hydrogen-bicarbonate co-production device. By adding alkaline electrolyte to the anode, we achieved a higher peak power density of 63 mW cm −2 at the corresponding hydrogen production rate of 0.57 mL min −1 cm −2 . More interestingly, the concentrations of pure NaHCO 3 solution can be controlled by adjusting the cathode water flow rate and fuel cell discharge current density. This work presents a theoretically feasible avenue for coupling hydrogen production and CO 2 utilization.
研究领域:
能源化学
·
电化学工程
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环境科学
·
可持续能源
·
碳捕集与利用
·
氢能技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Junshen Zhang,Juan Luo,Jiashan Chen,Ziyan Xu,Yuyu Chen,Han Yan,Rui Ma,Shichang Sun
MgO’s great potential for capturing CO 2 has drawn a lot of attention, but the limited O 2– sites prevents its further development. This work proposed a microwave-induced method (microwave hydrothermal and microwave sintering) to produce high-performance MgO CO 2 adsorbent and was further modified using carbonates (K 2 CO 3 ) and nitrates of alkali metals (NaNO 3 , KNO 3 ). The outcomes demonstrated that the small particle size MgO nanocrystals (6.20 nm) with a CO 2 uptake of 1.8 mmol·g −1 could be produced by a unique method of microwave heating from the inside out. Among the modified samples, addition of 20 mol% NaNO 3 on the surface of MgO exhibited the highest CO 2 uptake (11.91 mmol·g −1 ), and the uptake was still 7.9 mmol·g −1 after 10 cycles. The addition of molten salt changed the adsorbent’s active sites, resulting in an increase in O 2– alkaline sites and the activation of MgO lattice defects, both of which improved the sample’s CO 2 adsorption performance. This work could offer a new idea for creating affordable and effective CO 2 solid adsorbents to capture CO 2 .
研究领域:
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 MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Luyue Wang,Yuzhu Chen,Zhengyang Xing,Jie Ma
Real-time monitoring of metal ion species and concentrations in water is a highly active research field. In the paper, a novel fluorescent molecule, (E)-N'-((5-(9-phenyl-9H-carbazol-3-yl) thiophen-2-yl) methylene) terephthalohydrazide (PCTMT), is synthesized via Suzuki reaction and Schiff-base reaction in turn. In the DMF-H 2 O (70 % v/v) solvent system, the PCTMT presents a good aggregation-induced enhancement (AIE) fluorescent effect and good selectivity and anti-interference for monitoring Co 2+ and Cu 2+ in water with a wide pH range. The probe's detection limit (LOD) reached 28.2 nM and 38.7 nM for Co 2+ and Cu 2+ , respectively. The binding constants between PCTMT and Co 2+ and Cu 2+ are calculated as 1.8 ×10 17 M -2 and 2.3 ×10 16 M -2 , at a 2:1 mol ratio. In the probe system, Co 2+ and Cu 2+ can be distinguished by oxalate titration. The detection mechanism is discussed through testing analyses with the theoretical simulation calculation via the density functional theory (DFT) and time-dependent density functional theory (TD-DFT). The probe also indicates good detection capacities in real water samples. This study may promote the development of coordinated-type ion probes and innovation in water quality detection technology.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 5
·3146-3157
·
IF 3.9
Yanlong Hu,Qiang Wang,Dingkai Hu,Yingshuang Zhang,Muhammad Furqan,Shijian Lu
Monoethanolamines (MEAs) are widely used for CO2 capture, but their regeneration energy consumption is very high. CO2 Phase change absorbents (CPCAs) can be converted into CO2-rich and CO2-lean phases after absorbing CO2, and the regeneration energy consumption can be reduced because only the CO2-rich phase is thermally desorbed. In this paper, a novel CPCA with the composition “MEA/n-butanol/H2O (MNBH)” is proposed. Compared with the reported MEA phase change absorbent, the MNBH absorbent has higher CO2 absorption capacity, smaller absorbent viscosity and CO2-rich phase volume. The MNBH absorbent has the highest CO2 absorption capacity of 2.5227 mol CO2 per mol amine at a mass ratio of 3 : 4 : 3. The CO2 desorption efficiency reaches 89.96% at 120 °C, and the CO2 regeneration energy consumption is 2.6 GJ tCO2−1, which is about 35% lower than that of the 30 wt% MEA absorbent. When the mass ratio of MNBH absorbent was 3 : 6 : 1, the CO2 recycling capacity was 4.1918 mol CO2 L−1, which is 76% higher than that of the conventional 30 wt% MEA absorbent. The phase change absorbent developed in this paper can reduce the desorbent volume by about 50% and has good absorption performance for CO2 in flue gas.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Gas Science and Engineering
·
2024
·
IF 0
Xuebi Du,Dawei Shao,Yinhua Wan
Metal-organic frameworks (MOFs) have shown potential as nanofillers for the selective capture of specific gases in mixed matrix membranes (MMMs). This study introduces an efficient method, utilizing a mild (100 °C) reaction condition and a short reaction time (20 min), for the synthesis of MOF-808(Ce) nanocrystals. The MOF-808(Ce) that is obtained exhibits porous characteristics, a notable affinity for CO 2 , and robust intermolecular interactions with PIM-1. Furthermore, this study pioneers the incorporation of MOF-808(Ce) as a filler into PIM-1, with varying loadings, to create PIM/MOF-808 MMMs for the purpose of CO 2 separation. Consequently, the MMMs containing 2 wt% MOF-808(Ce) demonstrate high CO 2 permeability of 6854 Barrer and CO 2 /N 2 selectivity of 23.2, which is far surpasses 2008 upper bound from Robeson and approaches the refined 2019 upper bound from MeKenow. A comparative analysis demonstrates the efficacy of MOF-808(Ce) as a filler in PIM-1 for the purpose of CO 2 separation.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
CHEMIE INGENIEUR TECHNIK
·
2021
·
IF 1.672
Taotao Ji,Liangliang Liu,Lingyi Wang,Yanshuo Li,Yi Liu
The practical application of membrane separation, such as CO 2 recovery from flue gas, is usually accompanied by harsh operating conditions of high temperature and pressure as well as acidic and humid feed properties, which poses a great challenge to the stability of membrane materials. In this work, zirconium phosphate material with highly stable porous-framework structure was synthesized by ionothermal method, and then, its incorporation into the polymer matrix to prepare ZrPOF-Pebax mixed-matrix membranes (MMMs) was pioneered. Benefiting from their 4.0 × 3.0 Å 7-ring windows and CO 2 -philic framework, the optimal MMMs with a 5 wt % ZrPOF content exhibited enhanced CO 2 /N 2 selectivity of 29.6, with a decent CO 2 permeability of 286.3 Barrer, which raised by 79.4 and 67.5% compared to the neat Pebax 2533 membranes, respectively. Furthermore, owing to their excellent thermal, water, and chemical stability, obtained MMMs maintained excellent performances under harsh operating conditions.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zhuoxue Li,Yunlei Shi,Yimian Ding,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Xiaopeng Xuan,Jianji Wang
A Pickering emulsion is a natural microreactor for interfacial catalysis in which an emulsifier is critical. Recently, a metal–organic framework (MOF) has attracted attention to emulsify water–organic mixtures for constructing a Pickering emulsion. However, a few stimuli-responsive Pickering emulsions based on MOFs have been reported, and the MOF emulsifiers cannot be regenerated at room temperature. Herein, the Zr-MOF with a rodlike morphology is synthesized using ionic liquid as a modulator and then modified with n-(trimethoxysilylpropyl)imidazole (C3im) to prepare a series of functionalized Zr-MOFs (MOF-C3im). It is found that MOF-C3im is an excellent emulsifier to construct stable and CO2-responsive Pickering emulsions even at low content (>0.20 wt %). Notably, the emulsification and demulsification of the emulsions can be easily and reversibly switched by bubbling of CO2 and N2 alternatively at room temperature because CO2 and imidazole molecules anchored on the Zr-MOF underwent a reversible acid–base reaction, resulting in an obvious change in the wettability of the emulsifier. As a proof of concept, the reduction reactions of nitrobenzene have been successfully carried out in these Pickering emulsions, demonstrating the efficient integration as a microreactor for chemical reaction, product separation, and emulsifier recycling under ambient conditions. This strategy provides an innovative option to develop stimulus-responsive Pickering emulsions for sustainable chemical processes.
研究领域:
材料科学
·
化学工程
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）