SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Guangcan Huang,Tongxin Liu,Haoxin Peng,Yabo Xie,Qiang Chen,Jian-Rong Li
Mixed-matrix membranes (MMMs) incorporating Metal-Organic Frameworks (MOFs) represent a promising approach for gas separation, which can combine the advantages of selective adsorbents and processable polymers, and display great potential in the gas separation process. However, the further application of MMMs is severely impeded owing to the non-ideal interface between fillers and polymer matrix . In this work, a series of MIL-101(Cr) nanofillers, equipped with different kinds of counter anions were introduced to regulate the chemical microenvironment of the MMMs and improve the interfacial relationship between inorganic filler and polymer. The filler of MIL-101-HNO 3 exhibits improved dispersibility in solvents and heightened interface relationship with the polymer matrix (PIM-1) due to its optimal particle size and distinctive exposure of crystallographic planes. Moreover, gas sorption isotherms reveal that the MIL-101-HNO 3 MOF show reduced N 2 adsorption capacity. Therefore, the MOF filler of MMMs were optimized rationally by microenvironment regulate strategy, leading to the MIL-101-HNO 3 /PIM-1 MMMs achieve high CO 2 permeability and exceptional CO 2 /N 2 ideal selectivity (CO 2 = 14879 barrer, CO 2 /N 2 = 24.3), surpassing the latest 2019 upper bound. That makes MIL-101-HNO 3 /PIM-1 a potential candidate for the selective removal of CO 2 from stack gas and provides new insights into the regulation of the MMMs nanofiller microenvironment.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Yutong Pan,Pengju Gao,Shixiong Tang,Xiaoyu Han,Ziwen Hao,Jiyi Chen,Zhenmei Zhang,Heng Zhang,Xiaohui Zi,Maoshuai Li,Shiwei Wang,Yue Wang,Xinbin Ma
This work synthesized a series of Ni/CeO 2 /Al 2 O 3 catalysts with varying CeO 2 doping amounts to enhance low-temperature CO 2 methanation. The introduction of CeO 2 weakens the interaction between Ni and Al 2 O 3 , leading to the formation of Ni-CeO 2 active sites. This results in a high dispersion of Ni and CeO 2 , improved catalyst reducibility, increased number of active sites, and enhanced the CO 2 methanation. This work further investigated the impact of WHSV and catalyst stacking configuration to enhance the reaction. When the catalyst is stacked into three segments with a temperature gradient of 330 °C, 300 °C, and 250 °C under WHSV=9000 ml·h –1 ·(g cat) –1 , the CO 2 conversion significantly increases to 95%, which is remarkably close to the thermodynamic equilibrium (96%).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chen Wang,Yan Zhu,Ling Zhao,Rui Wang,Jun Jin,Yansheng Gong,Huanwen Wang,Beibei He
Solid oxide electrolysis cells (SOECs) have emerged as a promising technology for CO 2 electrolysis. However, the sluggish kinetics of CO 2 electrolysis impedes their widespread commercialization. Here, a novel heterostructure of in-situ exsolved metal/high-entropy perovskite, Ni@Sr 2 Fe 1.0 Ti 0.2 Cr 0.2 Mn 0.2 Mo 0.2 Ni 0.2 O 6-δ (Ni@SFTCMMN), has been designed to enhance the efficiency of CO 2 electrolysis. The Ni@SFTCMMN, with its high-entropy configuration and embedded exsolution morphology, ensures high structural stability during continuous CO 2 electrolysis. As an application, the Ni@SFTCMMN-based electrolysis cell demonstrates a remarkable current density of 1.91 A cm −2 at 1.5 V and 800 °C, maintaining consistent performance over 160 h. By integrating theoretical calculation with experimental investigations, we aim to establish the link between the electronic structure of perovskite oxides with varying elemental compositions and the mechanism of the CO 2 reduction reaction. The findings from this work provide crucial insights into the role of conformational entropy strategies in CO 2 electrolysis and suggest potential pathways for developing efficient and durable cathode of SOECs.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Muhammad Sabir,Mahmoud Sayed,Zhuofan Zeng,Bei Cheng,Wang Wang,Chuanbin Wang,Jingsan Xu,Shaowen Cao
The photocatalytic conversion of carbon dioxide (CO 2 ) into valuable products holds great promise from environmental and economic perspectives. However, current photocatalytic materials still exhibit unsatisfactory efficiency. In this study, a notably efficient step-scheme (S-scheme) heterojunction was developed by combining the Co-MOFs with carbon nitride nanosheets (g-C 3 N 4 ). The electrostatic interaction between these components not only facilitates the exfoliation of g-C 3 N 4 layers but also enhances the stability of the photocatalyst structure. The optimal heterojunction Co-CN4 photocatalyst achieved a significantly enhanced CO production rate of 16.1 µmol g −1 h −1 , which is 4.7 times higher than that of pure g-C 3 N 4 . This improved activity is ascribed to the enhanced light absorption and mitigated charge carrier recombination. Density functional theory (DFT) computations in conjunction with experimental observations elucidate the establishment of a close contact interface. Additionally, electron paramagnetic resonance (EPR) and in situ X-ray photoelectron spectroscopy (XPS) characterization unveil the electron transfer pathway of Co-CN4 during photocatalytic CO 2 conversion. This study offers valuable insights into the design of S-scheme photocatalysts for enhancement of CO 2 photoreduction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yuying Zhao,Shengchun Hu,Qixin Yuan,Ao Wang,Kang Sun,Ziyun Wang,Mengmeng Fan,Jianchun Jiang
Electrochemical CO 2 conversion into formate by intermittent renewable electricity, presents a captivating prospect for both the storage of renewable electrical energy and the utilization of emitted CO 2 . Typically, Cu-based catalysts in CO 2 reduction reactions favor the production of CO and other by-products. However, we have shifted this selectivity by incorporating B, N co-doped carbon (BNC) in the fabrication of Cu clusters. These Cu clusters are regulated with B, N atoms in a porous carbon matrix (Cu/BN-C), and Zn 2+ ions were added to achieve Cu clusters with the diameter size of ∼1.0 nm. The obtained Cu/BN-C possesses a significantly improved catalytic performance in CO 2 reduction to formate with a Faradaic efficiency (FE) of up to 70 % and partial current density (j formate ) surpassing 20.8 mA cm −2 at −1.0 V vs RHE. The high FE and j formate are maintained over a 12-hour. The overall catalytic performance of Cu/BN-C outperforms those of the other investigated catalysts. Based on the density functional theory (DFT) calculation, the exceptional catalytic behavior is attributed to the synergistic effect between Cu clusters and N, B atoms by modulating the electronic structure and enhancing the charge transfer properties, which promoted a preferential adsorption of HCOO* over COOH*, favoring formate formation.
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PubMed
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ChemSusChem
·
2024
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IF 7.5
Chen Liao,Hongwei Zhou,Shunxin Zhang,Feng Wang,Ya Liu,Liejin Guo
Graphical A highly effective photocatalytic system (V Cu −CuInS 2 /MXene) was developed for transforming CO 2 into acetate under full spectrum irradiation. The incorporation of the LSPR effect and defect engineering leads to a highly selective system. Photocatalytic CO 2 conversion towards C 2+ fuels is a promising technology for simultaneously achieving carbon neutrality and alleviating the energy crisis. However, this strategy is inefficient due to the difficulty of both multi-electron transfer and C−C coupling during C 2+ formation. In this work, CuInS 2 /MXene heterostructure with Cu vacancy is rationally designed by in situ hydrothermal synthesis. The V Cu −CuInS 2 /MXene heterostructure has a suitable band structure and tight interface contact. Catalytic performances under different testing conditions, in situ spectroscopy, and COMSOL simulation reveal that LSPR-activated MXene promotes the formation of crucial intermediate CH 2 * and triggers the C−C coupling process under near-infrared light, as the key to acetate. Moreover, in situ XPS analysis, DFT calculations, and photoelectrochemical characterizations unveil that copper vacancy can promote charge transfer from CuInS 2 to MXene and boost local electron aggregation on the MXene, further enhancing the photocatalytic efficiency and selectivity of C 2 products. Contributing to the synergistic effect of copper vacancy and plasmonic MXene, V Cu −CuInS 2 /MXene achieved excellent CO 2 RR activity with an acetate evolution rate of 250.0 μmol/h/g and a selectivity of 97.5 % under the full spectrum irradiation, which is 38.8 and 3.3 times higher than that of V Cu −CuInS 2 and CuInS 2 /MXene, respectively.
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Coatings
·
2024
·Vol. 14
·期 4
·383
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IF 2.9
Chunling Xin,Shufen Hou,Lei Yu,Xiaojing Zhou,Yunkai Fu,Xiaoteng Yang,Weiwei Sun,Fan Yang,Xia Wang,Lili Liu
Yellow nanorod Mg-MOF-74 was obtained through a solvothermal synthesis method. The XRD, N2adsorption–desorption isotherms, SEM, and TGA results suggest that the particle size of Mg-MOF-74 reaches 400 nm after the introduction of sodium acetate in the precursor of Mg-MOF-74. Furthermore, the morphology of Mg-MOF-74 changed from cauliflower- to rod-shaped particles. At the same time, the BET specific surface area and pore volume of Mg-MOF-74 also increased a lot. Then, the CO2dynamic adsorption capacity of Mg-MOF-74 was measured with a self-made fixed bed at 30 °C and a 0.1 bar CO2partial pressure. The results show that the CO2adsorption capacity of Mg-MOF-74-N2 reaches 3.67 mmol/g, and its CO2adsorption capacity remains unchanged after 10 CO2adsorption–desorption cycles.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Jiawei Dai,Deyu Zhu,You Xu,Jiannan Zhu,Xiaoling Liu,Guichan Xu,Zhengyun Wang,Rong Chen,Hongfang Liu,Guangfang Li
An efficient electrocatalytic conversion of CO2 into valuable multicarbon (C2+) products requires enhanced C–C coupling of C1 intermediates. Herein, we combine a tandem effect with a confinement strategy to construct a hollow Cu2O@Ag nanoshell electrocatalyst with a well-defined porous structure to improve the *CO intermediate coverage on the catalyst surface. In CO2 electroreduction, in situ Raman spectroscopy shows that the introduction of Ag can not only promote the CO intermediate production but also improve the stability of Cu+ to capture the *CO intermediate due to a CO-tandem effect, and the fine-tuned hollowness degree and pore size of Cu2O@Ag create a spatially confined microenvironment for trapping CO2 as well as the enrichment of CO, which greatly facilitate subsequent C–C coupling for C2+ product. The optimized Cu2O@Ag-45 with a specific nanoconfinement exhibits an enhanced ethylene (C2H4) production under the wide potential range from −0.4 to −1.2 V (vs RHE), and a Faradaic efficiency of 55.4% for C2+ products could be achieved at −1.2 V (vs RHE). This study highlights a promising strategy for the electrochemical reduction of CO2 to C2+ products on efficient C–C coupling catalysts.
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ACS Sustainable Chemistry & Engineering
·
2017
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IF 5.951
Yan Gao,Lu Ye,Shuyan Cao,Hu Chen,Yanan Yao,Jian Jiang,Licheng Sun
Perovskite hydroxide CoSn(OH)6 nanoparticles were synthesized and used for the first time in the photocatalytic reduction of CO2 to CO. Under mild reaction conditions and using [Ru(bpy)3](PF6)2 as the photosensitizer, a high photocatalytic efficiency of 19.3 μmol for CO evolution with a high selectivity of 86.46% was obtained. The photocatalytic activity and CO selectivity were further improved by adding weak Brönsted acids, as proton sources, to the system.
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ENERGY & FUELS
·
2017
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IF 3.091
Ke Wang,Wei Li,Zeguang Yin,Zhongyun Zhou,Pengfei Zhao
A sodium chloride (NaCl) doping–hydration technique was used to modify the structure of Li4SiO4 to improve its sorption properties at a low CO2 concentration. X-ray diffraction, nitrogen adsorption, scanning electron microscopy, X-ray photoelectron spectroscopy, differential scanning calorimetry, and thermogravimetric analyses were conducted to characterize the compositions, textural characteristics, morphologies, chemical valence states, molten phases, and adsorption properties of the synthesized samples. Hydration and NaCl doping produced synergistic effects. On one hand, a small particle size and large specific surface area were obtained, significantly facilitating chemisorption processes. On the other hand, co-doped sodium and chlorine induced molten phases when absorbing CO2, noticeably decreasing CO2 diffusion resistance. Thus, the CO2 absorption rate and uptake were remarkably improved. Different amounts of NaCl also greatly affected the morphology and chemisorption properties of the sorbents. At the optimized NaCl concentration, the sorbent only required 3 wt % doping to attain a maximum sorption capacity of up to 34.2 wt %. Moreover, the high capacity was maintained after 10 sorption/desorption cycles.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2017
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IF 3.615
Jun Liu,Yunfei Liu,Xiaowei Jiang,Yali Luo,Yinong Lyu
Two kinds of POSS-based microporous organic polymers (PMOPs) were prepared by cost-effective Friedel-Crafts reaction of octaphenylsilsesquioxanes with p -dimethoxybenzene (PMOP-1) or cyanuric chloride (PMOP-2). PMOP-1 with high surface area of 806 m 2 g −1 exhibited reasonable CO 2 adsorption (2.59 mmol g −1 , 273 K/1 bar) and selectivity, whereas PMOP-2 with lower surface area (559 m 2 g −1 ) showed a higher CO 2 /N 2 selectivity (30.0) and CO 2 /CH 4 selectivity (6.8) at 273 K/1 bar due to the high amount of nitrogen incorporated within the structure. The correlation between the performance of PMOPs in CO 2 capture/separation and their properties such as surface area, surface active sites, and heat of adsorption was investigated. The combination of a cost-effective method, high thermal stability, and reasonable selective adsorption make these materials potential candidates for application in CO 2 capture and separation technology.
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CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Shikai Liu,Chuqiao Shi,Chaokai Xu,Haichuan Zhang,Wenqi Li,Valentín Briega-Martos,Qian He,Yimo Han,Yao Yang
CO2 reduction reaction (CO2RR) facilitates the sustainable synthesis of fuels and chemicals. Although copper (Cu) enables CO2-to-multicarbon product (C2+) conversion, Cu-based electrocatalysts, particularly nanocatalysts, face challenges in poor selectivity and stability owing to the highly dynamic nature of Cu atoms under reaction conditions. Core–shell structures present a promising approach to address these issues by modulating the Cu overlayer–substrate interactions with atomic-level precision. Here, we report on Pd@Cu core–shell structures with atomically thin and nanometer-thick Cu overlayers on single-crystal Pd nanocubes with {100} facets promoting the CO2-to-C2+ conversion. The microstructures and surface compositions at the atomically sharp Pd/Cu interface were investigated by atomic-scale scanning transmission electron microscopy (STEM) imaging and electron energy-loss spectroscopy (EELS). Our results reveal that atomic-layer Cu epitaxially grows on Pd and adapts to the lattice of the Pd substrate. The reaction-driven migration of atomic-layer Cu is effectively suppressed on Pd due to the strong Cu–Pd interaction. While Pd only reduces CO2 to C1 products, atomic-layer Cu on Pd can initiate the C2+ production during the CO2RR. Thick Cu overlayers (∼15 nm) on Pd further enhance the C2+ faradaic efficiency while undergoing significant structural reconstruction, with only the 2–3 nm Cu layers near the Pd surface remaining stable and resistant to Cu migration after the CO2RR. We anticipate that Pd@Cu core–shell structures with intermediate Cu shell thickness hold significant potential for enhancing C2+ selectivity while maintaining high stability of nanocatalysts for CO2 reduction to liquid fuels.
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