CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2025
·
IF 3.9
Xingyu Lin,Hongsheng Lu,Ruoxin Zhang,Yingjiang Chen,Baiwen Huang
Gas channeling during CO 2 flooding presents a significant challenge to the effective underground storage of CO 2 . This study introduces a novel gas channel blocking strategy using the phase transition properties of fatty acid based CO 2 -responsive ionic liquids (ILs). The ILs were synthesized from choline hydroxide (Ch) and high-melting-point fatty acids (FA), including myristic acid (C14) and palmitic acid (C16), named FA-Ch ILs. These ILs demonstrate phase transformation behavior after CO 2 injection, leading to the precipitation of FA as solid particles. The FA-Ch ILs aqueous solution exhibits low viscosity, ensuring excellent injectivity for oilfield applications. After CO 2 injection, the precipitated FA particles act as gas channeling plugging agents, while the protonated Ch ions effectively inhibit clay swelling to enhance oil recovery with a synergistic effect. Structural properties and interaction mechanisms of the FA-Ch system were characterized by FT-IR, 1 H NMR, and molecular dynamics simulations. The particle size of the FA precipitates was regulated by adjusting FA-Ch concentration and CO 2 injection rate to make it suitable as a profile control agent. Furthermore, Ch + ions demonstrate clay swelling inhibition comparable to traditional inhibitors like KCl. This dual-functionality positions FA-Ch ILs as an innovative solution for addressing gas channeling and clay swelling in CO 2 flooding, offering a cost-effective and environmentally friendly alternative to conventional methods.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
ZhiWei Dong,YaLing Jia,Zeyu Wang,Antony Rajendran,Wen-Ying Li
Electrocatalytic CO2 reduction to formic acid is a promising strategy to obtain value-added chemicals and achieve the carbon cycle. However, its practical application is generally impeded by the limited accessibility of CO2 to the catalyst's surface and the lack of efficient universal catalyst across different pH levels. Herein, we report a new catalyst, i.e., SnS2 decorated with hydrophobic polymer polyvinylidene fluoride (SnS2+PVDF), for the effective electrocatalytic CO2 reduction to formate/formic acid across a wide pH range in a flow cell. This catalytic system accomplishes a remarkable Faradaic efficiency for the formic acid production in alkaline (98%), neutral (86%), and acidic (93%) electrolytes. Also, the single-pass carbon efficiency reaches up to 72.77% in acidic electrolyte. Water contact angle measurements in association with the in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy results indicate that the inclusion of PVDF creates a hydrophobic microenvironment which increases the CO2/H2O ratio near the surface of SnS2 particles. As a consequence, SnS2 particles enjoy the enhanced CO2 concentration around their surface to form many three-phase (solid-liquid-gas) boundary. In-situ Raman spectra combined with electrocatalytic studies reveal that SnS2 undergoes reconstitution to form catalytically active Sn/SnS2 during the reaction. These findings ensure and expand the generality of hydrophobic microenvironment regulation strategy in promoting electrocatalytic CO2 reduction to formic acid.
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Energy Technology
·
2021
·Vol. 9
·期 8
·2100205
·
IF 3.631
Zipeng Zeng,Aya Gomaa Abdelkader Mohamed,Xiang Zhang,Yaobing Wang
Although metal–N-doped carbons are promising electrocatalysts for CO 2 -to-CO conversion due to their high conversion efficiency and current density, their commercial application is still challenging due to their narrow potential/current range. In general, a wide potential/current electrocatalyst is in high demand for industrial CO 2 electrocatalysis. Controllable strategy to tune N configurations toward pyridinic-enriched metal–N x active sites is attractive. The synergetic effect of the ability of pyridinic N to capture Lewis acidic CO 2 and the characteristics of Ni–N active sites to inhibit the hydrogen evolution reaction (HER) can achieve a wide potential window, which has high practical value. Herein, the well-chosen precursors resulting in a pyridinic-enriched Ni–N x site can selectively catalyze CO 2 toward CO generation in aqueous media with a high Faradaic efficiency (FE) of 100% with an overpotential of 680 mV. Continuous CO FE > 90% was recorded under a wide range of potentials without decay. Motivated by its practical characteristics in CO 2 electrocatalysts, a Zn–CO 2 battery is assembled achieving a CO 2 –CO conversion efficiency of more than 90% in a wide discharge current window. Therefore, the results highlight that pyridinic-enriched Ni–N x holds great promise as simultaneous CO-selective electrocatalyst by suitably tuning M–N configurations as new perspective strategy.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Xi Chen,Zhenggang Wang,Zhuo Yang,Guozhen Liu,Guining Chen,Gongping Liu,Xiuxia Meng,Naitao Yang,Wanqin Jin
Towards natural gas purification , polymeric membranes generally face challenges of trade-off between permeability and selectivity , as well as CO 2 -induced plasticization effect. Previous works demonstrated that incorporating high-performing nanofillers and crosslinking the polymers are effective methods to overcome these two issues, respectively. In this work, we aimed to simultaneously improve permeability, selectivity and plasticization resistance of polymeric membranes by incorporating surface-engineered nanoporous fillers for CO 2 /CH 4 separation. DD3R zeolite nanoparticles with high purity were synthesized and then surface-functionalized by 3-aminopropyl trimethoxysilane (APTMS) to serve as the filler. Mixed-gas permeation measurements showed that DD3R zeolites offered CO 2 -selective channels in 6FDA-DAM polyimide based on molecular sieving effect of zeolitic aperture. 30 wt% DD3R-APTMS zeolite imparted the membrane with CO 2 permeability of 1661 Barrer (increased by 71.7%) and CO 2 /CH 4 selectivity of 28.0 (increased by 44.5%), which was beyond the upper-bound of polymeric membranes. Meanwhile, the hydrogen bond interaction between amino groups on APTMS and carboxyl groups on 6FDA-DAM rendered the resulting DD3R-APTMS MMMs highly enhanced plasticization resistance over 40 bar when equimolar CO 2 /CH 4 mixture as the feed. This work demonstrates a facile approach to simultaneously enhance separation performance and mitigate the plasticization effect.
研究领域:
材料科学
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化学工程
·
膜技术
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JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Leixin Yang,Shengbo Zhang,Hong Wu,Chumei Ye,Xu Liang,Shaofei Wang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Yutao Liu,Nayab Nasir,Zhongyi Jiang
For high-performance mixed-matrix membranes (MMMs), it is crucial to design gas transport channels in fillers to rationally manipulate the structure-property relationship. In this study, the novel porous organosilicon nanotubes (PSiNTs) were incorporated into Pebax to prepare MMMs for biogas purification (CO 2 /CH 4 separation). After comparing the separation performance of MMMs containing PSiNTs and MMMs containing non-porous organosilicon nanotubes (SiNTs),it can be found that the porous structure on wall of organosilicon nanotubes had a significant effect on the improvement of the gas permeability . In addition, the amino-modified PSiNTs (N-PSiNTs) were prepared and introduced into membranes to significantly enhance the CO 2 permeability and CO 2 /CH 4 selectivity. Firstly, the porosity of N-PSiNTs afforded rapid gas transport channels in MMMs and intensified the diffusion mechanism, increasing the CO 2 permeability. Secondly, the reversible reaction between amino groups and CO 2 in MMMs intensified the facilitated transport mechanism, increasing the CO 2 /CH 4 selectivity. In particular, the Pebax-N-PSiNTs with 0.5 wt% and 1 wt% N-PSiNTs exhibited the optimal separation performance, which surpassed 2008 upper bound and were superior to the MMMs incorporated with other kinds of nanotubes.
研究领域:
材料科学
·
环境工程
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ying Cheng,Shumaila Razzaque,Zhen Zhan,Bien Tan
Fabrication of functionalized hypercrosslinked polymers (HCPs) with high specific surface area has gained significant research interest and their utilization for gas storage is still a trending research area. Considering the significance of solvent knitting strategy in construction of remarkably high surface area HCPs, we report fabrication of cyano-functional HCPs via one step Friedel-Crafts reaction. The series of HCPs were obtained by copolymerizing the rigid monomer TPB with a 2-napthonitrile in different molar ratio. The resultant co-polymerized polymers contained a plenty of nitrile functional groups and possessed high BET surface area. Among the series of such HCPs, HCP-TPB-CN-3:1 showed the highest BET surface area up to 2017 m 2 g −1 . These HCPs have enriched nitrogen in their pore walls that enhance the facile interaction of CO 2 to achieve higher capture capacity of 21.3 wt% at 273 K. Moreover, the HCP-TPB-CN was explored for CH 4 storage and showed absolute adsorption capacity of 0.35 g/g at 273 K, 80 bar, which is comparable with the porous polymers reported so far. These results highlight the significance of solvent knitting strategy and broaden the scope of HCPs for versatile industrial applications.
研究领域:
材料科学
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化学工程
·
环境科学
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Advanced Energy Materials
·
2026
·
IF 25.5
Siyun Ren,Junnan Han,Jie Liang,Weixi Lu,Lin Zhou,Xing Zhang,Jun Xu,Jia Zhu
Solar-driven carbon dioxide (CO 2 ) hydrogenation represents a promising route for producing value-added chemicals/fuels with a negative carbon footprint. Plasmonic catalysis attracts significant attention as it synergistically employs thermochemistry and photochemistry, facilitated by multiple thermal and/or nonthermal effects, including efficient solar energy harvesting, localized heating, localized electric field, and hot carrier excitations. Herein, a metallic cobalt nanowire array is employed as the plasmonic catalyst to demonstrate that the reaction kinetics of CO 2 hydrogenation are effectively improved by light-excited plasmonic localized electric field through regulating the binding strength of reactive intermediates. Theoretical simulations and operando spectroscopic data further reveal that the catalytic durability is significantly enhanced compared to traditional thermocatalysis because of the localized electric field-assisted suppression of coking deactivation. This work presents the first demonstration of plasmonic-enhanced catalytic durability, delivering key mechanistic insights for the future design of efficient and stable plasmonic catalysts.
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高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
·
IF 5.141
Muhammad Bilal Akbar,Yanjie Wang,Xuehua Zhang,Tao He
Cu 2 O is an attractive photocathode for CO 2 reduction reaction (CO 2 RR). The instability of Cu 2 O usually makes it present as a part of composite or multilayer in CO 2 RR. The systematic study of pure Cu 2 O for CO 2 RR is quite rare, resulting in the elusiveness of the origin for the activity and selectivity of CO 2 RR under different conditions. Herein, exploration of the factors that influence the product distribution and Faradic efficiency of CO 2 RR using pure Cu 2 O is carried out, like Cu 2 O structure and electrolyte composition. Persistent Cu + is found to be key for selective CO 2 RR, especially favoring the formation of C2 product (CH 3 COOH). The Cu 2 O film thickness, local pH, and the electrolyte cations are revealed to influence the amount of surface Cu + . The number of H + and dissolved CO 2 affected by electrolytes also account for the disparity of CO 2 RR results. Therefore, by considering both the CO 2 RR and the dynamic change of Cu 2 O, this work has provided a compositional descriptor to link the structure of Cu 2 O and the CO 2 RR property, which can be useful for future development of Cu 2 O-based catalysts.
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Nano-Micro Letters
·
2022
·Vol. 14
·期 1
·1-13
·
IF 23.655
Ban Chaogang,Duan Youyu,Wang Yang,Ma Jiangping,Wang Kaiwen,Meng Jiazhi,Liu Xue,Wang Cong,Han Xiaodong,Cao Guozhong,Gan Liyong,Zhou Xiaoyuan
The g-C 3 N 4 isotype heterojunction was synthesized for photocatalytic CO 2 reduction, which exhibits an impressive activity and outstanding stability.
The isotype heterojunction presents more favorable charge separation and transfer performance than the single components.
The enhanced photogenerated charge dynamics in isotype heterojunction facilitates the production of key intermediates and thus the whole reaction kinetics.
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PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 19
·11426-11435
·
IF 4.22
Yan Dong,Peng Zhen,Wang Wei,Zeng Peng,Huang Yiyin
Abstract Carbon-based metal-free catalysts exhibit great applications in electrochemical CO 2 reduction (ECR), while most studies merely focus on large-sized carbons with limited ratio of surface atoms for engineering to create surface active centers. Here, we report a joint treatment of C60 by heating and plasma to induce a dramatic performance promotion during ECR. The electrochemical measurements indicate the Faraday efficiency for ECR toward CO production kept at high level over 80% in a wide potential region from − 0.4 to − 0.7 V versus RHE, with the highest value reaching 96.8%. The physical characterization reveals that fragmentation of C60 occurs together with N/O doping, both of which could induce change in electron structure, causing the formation of *COOH intermediate and ultimately leading to the optimized activity and selectivity for CO production. This treatment route was further revealed to be applicative for other carbon materials, e.g., single-walled carbon nanotube, to promote its ECR activity and selectivity. Graphical Abstract
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Lei Qinqin,Yuan Huiqing,Du Jiehao,Ming Mei,Yang Shuang,Chen Ya,Lei Jingxiang,Han Zhiji
The direct utilization of solar energy to convert CO 2 into renewable chemicals remains a challenge. One essential difficulty is the development of efficient and inexpensive light-absorbers. Here we show a series of aminoanthraquinone organic dyes to promote the efficiency for visible light-driven CO 2 reduction to CO when coupled with an Fe porphyrin catalyst. Importantly, high turnover numbers can be obtained for both the photosensitizer and the catalyst, which has not been achieved in current light-driven systems. Structure-function study performed with substituents having distinct electronic effects reveals that the built-in donor-acceptor property of the photosensitizer significantly promotes the photocatalytic activity. We anticipate this study gives insight into the continued development of advanced photocatalysts for solar energy conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Hongtao Ge,Zhengxiang Gu,Peng Han,Hanchen Shen,Abdullah M. Al-Enizi,Lijuan Zhang,Gengfeng Zheng
The increasing accumulation of CO 2 in the atmosphere has been leading to serious environmental problems. Electrochemical reduction of CO 2 is a potential means of carbon recycling for energy storage and environmental sustainability. However, it is limited by the lack of highly active and selective electrocatalysts. Here we demonstrate the development of mesoporous tin oxide (SnO 2 ) for electrocatalytic CO 2 reduction, which facilitates the adsorption and electrochemical reduction of CO 2 inside mesopores. The highly-ordered and uniform pore sizes of the mesoporous SnO 2 electrocatalyst favor the enhancement of formation of carbon monoxide (CO) and formate during the electrochemical reduction. The combined faradaic efficiencies of CO and formate reach a peak value of ∼80% at a current density of 5 mA cm −2 at −0.8 V vs. reversible hydrogen electrode. This work suggests attractive development of mesoporous electrocatalysts with a variety of pore size and structures for efficient energy conversion and electrochemical CO 2 reduction.
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