RARE METALS
·
2025
·
IF 11
Wang Long-Yan,Fan De-Qi,Li Yi,Zhao Cheng-Xiao,Yang Xiao-Fei
Metalloporphyrins featuring structurally tunable aromatic macrocycles and versatile metal coordination sites are widely recognized as promising molecular catalysts for photocatalytic carbon dioxide reduction. However, their catalytic performances are constrained by rapid recombination of photogenerated charge carriers, insufficient charge transfer efficiency, and structural instability caused by molecular aggregation. Anchoring metalloporphyrins onto conductive substrates, in particular ultrathin two-dimensional (2D) nanostructures, can effectively accelerate interfacial charge transport efficiency, thereby improving photocatalytic activity toward CO 2 reduction. In this work, a novel 2D/2D heterojunction was designed and synthesized, which can serve as a highly efficient molecular catalyst for visible-light-driven CO 2 reduction. The abundant Co centers and N-sites in the assembled cobalt-coordinated porphyrin nanobelts can greatly enhance the adsorption and conversion of CO 2 . Meanwhile, the presence of few-layer Ti 3 C 2 MXene nanosheets enables the accelerated interfacial charge transport from photoexcited metalloporphyrin to Ti 3 C 2 MXene. Rapid electron transfer is verified by Kelvin probe force microscopy (KPFM), in situ attenuated total reflectance-Fourier transform infrared (ATR-FTIR), and irradiated X-ray photonelectron spectroscopy (XPS). As expected, compared to pristine porphyrin, the metalloporphyrin/Ti 3 C 2 MXene heterojunction shows a 12.5-fold increase in the photocatalytic activity for CO 2 reduction to CO. Graphical abstract
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yang Zhang,Yue Zhang,Yilei Yan,Yuchao Ma,Kaihua Li,Shuo Yang,Long Jiao,Shaofei Wang,Bowen Cheng,Leixin Yang
Covalent organic frameworks (COFs) are promising membrane materials for gas separation due to their periodic pore structure and chemical tailorability. However, the COF membranes usually show oversized pores and a single separation mechanism, which limits their gas separation applications. In this work, we fabricate highly ordered covalent organic framework (COF) membranes through interfacial polymerization, guided by a nucleation–epitaxial growth mechanism that ensures dense and defect-free layers. By regulating monomer hydroxyl content and spatial distribution, we achieve tailored pore architectures and interlayer stacking. Furthermore, a microenvironment engineering strategy is implemented via post-modification with boric acid and piperazine, which fine-tunes the pore size and introduces CO 2 -philic sites, enabling a synergistic combination of diffusion selective and facilitated transport. The optimized membrane exhibits an evident pore contraction, with the average pore diameter decreasing from 2.04 nm to 1.06 nm, confirming the effective tuning of the internal channels. As a result, it delivers a high CO 2 permeance of 2149 GPU and a CO 2 /N 2 selectivity of 14.3. This microenvironment regulation approach reveals critical structure–property relationships and provides valuable guidance for the separation of small molecule mixtures by large-pore membrane materials.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Hanqing Lin,Ke Gong,Petr Hykys,Danke Chen,Wen Ying,Zdenek Sofer,Youguo Yan,Zhen Li,Xinsheng Peng
CO 2 separation and recovery technology is a significant part of resolving the global greenhouse issue. In order to develop a cost-effective and high-performance method to realize CO 2 separation, a new kind of supported liquid membrane was configured by incorporating deep eutectic solvent into the nanoslits of titanium carbide (Ti 3 C 2 T x ) membrane. The deep eutectic solvent is a novel ionic liquid analogous with equal physical and chemical advantages but more economical and environmental benign. And the Ti 3 C 2 T x , as a neoteric two-dimension material, can serve as a valid platform for supporting the deep eutectic absorbent. By combining the two kinds of material, the resultant Ti 3 C 2 T x supported deep eutectic liquid membrane shows good CO 2 preference against other light gases as well as high thermal stability and long-term durability. The permeance of CO 2 is about 26.35 GPU with selectivity over N 2 , CH 4 and H 2 are 319.15, 249.01 and 12.38, respectively. The molecule dynamic simulation is also applied to uncover the separation mechanism of CO 2 and the ingredient redistribution and interionic refactor phenomenon of deep eutectic solvent trapped in the Ti 3 C 2 T x nanoslits.
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DOI
高影响因子
Green Chemical Engineering
·
2020
·
IF 0
Weifang Zhu,Fu Liu,Minmin Gou,Ruili Guo,Xueqin Li
The two-dimensional (2D) nanosheet zinc cobaltate (ZnCo 2 O 4 ) was added into polyether block amide (Pebax) matrix to prepare mixing matrix membrane (MMM) for separating carbon dioxide (CO 2 )/methane (CH 4 ) gas mixture. The 2D porous ZnCo 2 O 4 nanosheets were composed of chemically interconnected metal oxide nanoparticles. The ZnCo 2 O 4 nanoparticles in the nanosheets constructed large-quantity pores of 11.78 nm and provided abundant transfer channels for gas molecule. Moreover, the synergistic effect of bimetallic Zn 2+ and Co 2+ would promote the generation of oxygen vacancies (O δ− ), which could provide more CO 2 (C δ+ ) adsorption sites, thereby increased the selectivity of the membrane. The large aspect ratio of the ultra-thin ZnCo 2 O 4 nanosheets showed better dispersion in the membrane. The pure gas separation performance data showed the CO 2 permeability and CO 2 /CH 4 selectivity of Pebax/ZnCo 2 O 4 membrane were 139.10 Barrer and 15.38, respectively, when the filling amount was 0.5 wt%. Compared with pure Pebax membrane, the separation performance (permeability and selectivity) were increased with 165.67% and 75.57%, respectively.
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DOI
ENVIRONMENTAL TECHNOLOGY
·
2021
·
IF 3.247
Wenwen Huang,Jiacheng Liu,Na Rao,Guozhi Fan,Juntao Yan,Qunpeng Cheng,Guangsen Song
Concerning the increasing greenhouse effect, the development of efficient CO2 adsorbents is very important. In this study, the influence of surfactant on the adsorption performance of amine-functionalized MCM-41 was analysed. The results showed that the residual amount of surfactant in MCM-41 was gradually decreased with the increase of calcination temperature which improved the pore structure. The maximum adsorption capacity (5.495 mmol/g) appeared at PEI-MCM-41-100°C indicated that the adsorption capacity could be improved under the function of surfactant. By calculating the diffusion coefficient of CO2 adsorption process in PEI-MCM-41-100/200/300/400/550°C, the diffusion resistance of CO2 was the lowest in PEI-MCM-41-100°C, which directly proved that the synergism of surfactant and organic amine could reduce the diffusion resistance of CO2 in the pore.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
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IF 3.141
Juzheng Song,Jie Liu,Wei Zhao,Yan Chen,Hang Xiao,Xiaoyang Shi,Yilun Liu,Xi Chen
Developing inexpensive and highly efficient CO2 air capture technologies is an important solution for solving the greenhouse problem. In this work, we used the low-cost quaternized chitosan (QCS)/poly(vinyl alcohol) (PVA) hybrid aerogels with quaternary ammonium groups and hydroxide ions to reversibly capture CO2 from ambient air by humidity swing. The CO2 capture capacity and adsorption rate of the aerogels were investigated over the temperature range 10–30 °C. The CO2 capture capacity of the aerogels was measured to be about 0.18 mmol/g, which is 38% higher than the state-of-the-art commercial membrane. In addition, we proposed a modified pseudo-first-order kinetic model considering both the CO2 adsorption and the H2O desorption, which describes the experimental results very well. For the first time, the moisture-swing CO2 adsorbent is built by low-cost biomass material, which opens up a new approach for the design of the moisture-swing CO2 adsorbent.
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DOI
高影响因子
Materials Research Express
·
2020
·Vol. 7
·期 3
·035026
·
IF 1.929
Qianxi Fang,Weiqiu Huang,Hongning Wang
SiO2 aerogels were prepared by sol-gel method and methyl alkylation reaction using TEOS as silicon sources. Silica-supported polyethylenimine (PEI/SiO2) adsorbents for CO2 adsorption were prepare by grafting techniques, in which mesoporous SiO2 aerogel was loaded with PEI and organic compounds functionalized by hydroxyl or amino groups as dopants. CO2 adsorption isotherms of PEI amine-modified SiO2 aerogels were measured and the results show that the maximum CO2 adsorption capacity (1.8 mmol g−1) was obtained over a doped SA-PEI-N-Y loaded with 45% PEI and 15% N-Y (N-[3-(Trimethoxysilyl)propyl]ethylenediamine, denoted as N-Y). In addition, SA-PEI-N-Y has stronger thermal stability than SA-PEI-60% in nitrogen from room temperature to 800 °C at a heating rate of 10 °C min−1. It turns out that N-[3-(Trimethoxysilyl)propyl]ethylenediamine is the best dopant.
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DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 4
·427
·
IF 4.501
Chen Qi,Somboon Chaemchuen,Meng Liu,Jichao Wang,Serge Zhuiykov,Francis Verpoort
Nitrogen-doped porous carbon material was generated via thermal pyrolysis of zeolitic imidazole frameworks (ZIFs). The structure of the ZIF templates was tuned, so that the obtained product was an N-doped porous carbon-containing encapsulated metal nanoparticle. The hierarchical structural and unique properties of pyrolyzed materials are involved in further application, including catalysis. The as-synthesized porous carbon materials were applied as a catalyst for CO2fixation on cyclic carbonates under near ambient pressure without solvent and co-catalyst. The zinc dispersion in highly porous carbon material, deriving from ZIF-8, exhibited a superior catalytic performance among the synthesized materials. The acid sites (Zn species) and the incorporated basic sites (N-species) present in the porous carbon material are essential for a high affinity for gas adsorption and CO2conversion. Additionally, the catalyst was found to be very robust and stable during recycling studies as the catalytic performance remained high for seven cycles.
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DOI
高影响因子
Journal of CO2 Utilization
·
2020
·
IF 5.993
Huan Wen,Lei Zhang,Yingjie Du,Ziyuan Wang,Yunhong Jiang,Hongjie Bian,Jiandong Cui,Shiru Jia
In this study, we synthesized for the first time a bimetal-based inorganic-carbonic anhydrase (CA) hybrid nanoflower to immobilize CA using Cu 2+ and Zn 2+ instead of single metal ion. Subsequently, the synthesized bimetallic hybrid nanoflowers (CANF) were embedded into the poly(vinyl alcohol) (PVA)-chitosan (CS) hydrogel networks to obtain PVA/CS@CANF hydrogel membrane. The CANF exhibited a significantly higher activity recovery of 70 % compared with 35 % with CA/Zn 3 (PO 4 ) 2 hybrid nanoflowers and 10 % with CA/Cu 3 (PO 4 ) 2 hybrid nanoflowers. The PVA/CS@CANF hydrogel membrane possessed excellent mechanical strength, high catalytic activity, and were easy to flow out without centrifugation or filtration. At the same time, the PVA/CS@CANF displayed higher thermostability, storage stability, and pH stability than free CA and CANF , and superior reusability and CO 2 capture capacity. The hydrogel membrane maintained more than 75 % of its original activity after 8 cycles. However, CANF only maintained 12 % of its original activity. Furthermore, the amount of CaCO 3 produced by PVA/CS@CANF membrane was 9.0-fold and 2.0-fold compared with free CA and CANF, respectively. Therefore, This approach to synthesizing bimetallic-based protein hybrid hydrogel membrane could have a bright future in CO 2 capture.
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DOI
高影响因子
ACS Nano
·
2021
·
IF 15.881
Peilong Lu,Xin Tan,Haitao Zhao,Qian Xiang,Kaili Liu,Xiaoxu Zhao,Xinmao Yin,Xinzhe Li,Xiao Hai,Shibo Xi,Andrew T S Wee,Stephen J. Pennycook,Xuefeng Yu,Menglei Yuan,Jianbo Wu,Guangjin Zhang,Sean C. Smith,Zongyou Yin
An atomically dispersed structure is attractive for electrochemically converting carbon dioxide (CO2) to fuels and feedstock due to its unique properties and activity. Most single-atom electrocatalysts are reported to reduce CO2 to carbon monoxide (CO). Herein, we develop atomically dispersed indium (In) on a nitrogen-doped carbon skeleton (In–N–C) as an efficient catalyst to produce formic acid/formate in aqueous media, reaching a turnover frequency as high as 26771 h–1 at −0.99 V relative to a reversible hydrogen electrode (RHE). Electrochemical measurements show that trace amounts of In loaded on the carbon matrix significantly improve the electrocatalytic behavior for the CO2 reduction reaction, outperforming conventional metallic In catalysts. Further experiments and density functional theory (DFT) calculations reveal that the formation of intermediate *OCHO on isolated In sites plays a pivotal role in the efficiency of the CO2-to-formate process, which has a lower energy barrier than that on metallic In.
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DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Zhong Changyin,Yang Yifei,Chen Jun,Feng Bomin,Wang Hongbing,Yao Yunxi
CO 2 methanation is regarded as an efficient method for upgrading CO 2 to fuels and reducing environmental impacts of greenhouse gas emission. In this study, we developed Ni/ La 2 O 2 CO 3 low temperature CO 2 methanation catalysts by tuning the metal-support interaction via changing the morphology of catalyst supports. La 2 O 2 CO 3 supports with various morphologies including nanotriangles (La 2 O 2 CO 3 -T), nanorods (La 2 O 2 CO 3 -R), and nanoparticles (La 2 O 2 CO 3 -P), were synthesized as the supports of Ni catalysts for CO 2 methanation reaction. The CO 2 methanation performance of the synthesized Ni/La 2 O 2 CO 3 catalysts was found to be markedly superior to that of conventional Ni/SiO 2 catalysts with the following orders: Ni/La 2 O 2 CO 3 -T > Ni/La 2 O 2 CO 3 -R > Ni/La 2 O 2 CO 3 -P > Ni/SiO 2 . In the comparative characterization of Ni/La 2 O 2 CO 3 catalysts with various morphologies, TEM and H 2 -TPR results reveal that the Ni/La 2 O 2 CO 3 -T catalysts exhibit better dispersion of Ni nanoparticles and higher reducibility. Moreover, X-ray photoelectron spectroscopy (XPS), O 2 and H 2 temperature programmed desorption (O 2 -TPD, H 2 -TPD) results indicate that the Ni/La 2 O 2 CO 3 -T catalysts possess a lower oxygen vacancy formation energy leading to a higher concentration of interfacial oxygen vacancies, which enhances the adsorption hydrogen at these interfacial oxygen vacancy sites. CO 2 -TPD results further reveal that Ni/La 2 O 2 CO 3 -T catalysts own higher concentration of medium basic sites, which promote the adsorption and activation of CO 2 . Consequently, Ni/La 2 O 2 CO 3 -T catalysts demonstrate superior low-temperature CO 2 methanation activity by hydrogenation of CO 2 adsorbed as surface carbonates on the La 2 O 2 CO 3 surfaces with hydrogen spilled over from the Ni surfaces via the interfacial oxygen vacancies to the catalyst support. Graphical Abstract
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DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 14
·8592-8599
·
IF 4.036
Yan Zhang,Ziqi Wei,Xing Liu,Fan Liu,Zhihong Yan,Shangyong Zhou,Jun Wang,Shuguang Deng
Biomass-derived porous carbons are regarded as the most preferential adsorbents for CO2 capture due to their well-developed textural properties, tunable porosity and low cost. Herein, novel porous carbons were facilely prepared by activation of palm sheath for the highly selective separation of CO2 from gas mixtures. The textural features of carbon materials were characterized by the analysis of surface morphology and N2 isotherms for textural characterization. The as-prepared carbon adsorbents possess an excellent CO2 adsorption capacity of 3.48 mmol g−1 (298 K) and 5.28 mmol g−1 (273 K) at 1 bar, and outstanding IAST selectivities of CO2/N2, CO2/CH4, and CH4/N2 up to 32.7, 7.1 and 4.6 at 298 K and 1 bar, respectively. Also, the adsorption evaluation criteria of the vacuum swing adsorption (VSA) process, the breakthrough experiments, and the cyclic experiments have comprehensively demonstrated the palm sheath derived porous carbons as efficient adsorbents for practical applications.
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DOI
高影响因子
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