Nano-Micro Letters
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2023
·Vol. 15
·期 1
·1-15
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IF 26.6
Li Minhan,Zhang Fangzhou,Kuang Min,Ma Yuanyuan,Liao Ting,Sun Ziqi,Luo Wei,Jiang Wan,Yang Jianping
Electrochemical reduction of CO 2 into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO 2 capture and utilization, resulting from their high catalytic activity and selectivity. The mobility and accessibility of active sites in Cu-based catalysts significantly hinder the development of efficient Cu-based catalysts for CO 2 electrochemical reduction reaction (CO 2 RR). Herein, a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride (g-C 3 N 4 ) as the active sites for CO 2 -to-CH 4 conversion in CO 2 RR. By regulating the coordination and density of Cu sites in g-C 3 N 4 , an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH 4 Faraday efficiency of 49.04% and produces the products with a high CH 4 /C 2 H 4 ratio over 9. This work provides the first experimental study on g-C 3 N 4 -supported single Cu atom catalyst for efficient CH 4 production from CO 2 RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO 2 RR by engineering Cu active sites in 2D materials with porous crystal structures.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2023
·Vol. 99
·期 1
·183-194
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IF 3.4
Zhen Wang,Zhitao Han,Gang Liu,Zelu Zhou,Xi Wu,Song Zhou,Xinxiang Pan
BACKGROUND The large-scale practical application of CO 2 capture using carbonate solutions is mainly limited by their low CO 2 absorption rate. In view of this, it is feasible to improve CO 2 capture performance of carbonate solution by adding additives. In this paper, low-cost sodium carbonate (Na 2 CO 3 ) solution was selected as the main CO 2 absorbent, and the effects of different organic additives on CO 2 capture performance of Na 2 CO 3 solutions were systematically investigated. RESULTS The results showed that 0.04 mol/L tetrabutylammonium bromide (TBAB) could achieve a better enhancement effect on CO 2 capture performance of Na 2 CO 3 solution. After addition of TBAB, the maximum CO 2 absorption rate of Na 2 CO 3 solution was improved to 2.52 × 10 −3 mol/min, which increased by 105%. And the maximum CO 2 desorption rate could also be improved by 45%. TBAB/Na 2 CO 3 system not only realized a high CO 2 absorption capacity of 0.769 mol/mol, but also maintained 82% of the initial CO 2 absorption capacity after three cyclic tests. The regeneration heat duty of TBAB/Na 2 CO 3 solution was calculated to be 1136.6 kJ/mol, which was significantly lower than that of single Na 2 CO 3 solution and conventional MEA aqueous solution. The promotion mechanism of TBAB in Na 2 CO 3 solution was explored using Fourier transform infrared spectra (FTIR) and 13 C nuclear magnetic resonance (NMR) analysis. CONCLUSION The introduction of TBAB additive could significantly improve CO 2 capture performance of Na 2 CO 3 solution and reduce regeneration heat duty, making it a possible option in the field of post-combustion CO 2 capture. © 2023 Society of Chemical Industry (SCI).
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Teng Lu,Zhaomin Li,Liping Du
This study explores the combined application of hydrophobic silica aerogels and SDS to enhance CO 2 storage capacity and oil recovery. Experimental data highlighted a marked increase in CO 2 solubility within silica aerogel-SDS nanofluids compared to brine and SDS solutions. Molecular dynamics simulations revealed CO 2 adsorption into nanopores. Silica aerogel nanoparticles extended CO 2 foam half-life by 6 % versus 62 % decline for sole SDS foam from 30 to 140 °C. Adjusting the SDS to nanoparticle ratio affects foam properties, with a ratio of 1.5 yielding optimal results. Core flooding experiments demonstrated a 75 % rise in CO 2 trapping efficiency using the nanofluids over SDS solutions. Two-dimensional tests showed aerogel-SDS foam surpassed SDS foam flooding by 12 % incremental oil recovery in upper layers, attributed to enhanced profile control. The combined agents present an effective approach for geological CO 2 storage and EOR optimization.
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ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Chenchen Qin,Li Xu,Jian Zhang,Jun Wang,Jiaxin He,Daomeng Liu,Jia Yang,Juan-Ding Xiao,Xifan Chen,Hong-Bao Li,Zhengkun Yang,Junzhong Wang
Electroreduction of carbon dioxide into readily collectable and high-value carbon-based fuels is greatly significant to overcome the energy and environmental crises yet challenging in the development of robust and highly efficient electrocatalysts. Herein, a bismuth (Bi) heterophase electrode with enriched amorphous/crystalline interfaces was fabricated via cathodically in situ transformation of Bi-based metal-phenolic complexes (Bi-tannic acid, Bi-TA). Compared with amorphous or crystalline Bi catalyst, the amorphous/crystalline structure Bi leads to significantly enhanced performance for CO2 electroreduction. In a liquid-phase H-type cell, the Faraday efficiency (FE) of formate formation is over 90% in a wide potential range from −0.8 to −1.3 V, demonstrating a high selectivity toward formate. Moreover, in a flow cell, a large current density reaching 600 mA cm–2 can further be rendered for formate production. Theoretical calculations indicate that the amorphous/crystalline Bi heterophase interface exhibits a favorable adsorption of CO2 and lower energy barriers for the rate-determining step compared with the crystalline Bi counterparts, thus accelerating the reaction process. This work paves the way for the rational design of advanced heterointerface catalysts for CO2 reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xiaohong Ma,Jiajia Zheng,Huacheng Jin,Xi Zeng,Danyang Li,Feifei You,Jian Qi,Fangli Yuan
The utilization of solar energy to convert CO 2 into small energy molecules is a potential “carbon neutral” technology for CO 2 emission reduction. However, the industrial application is significantly constrained due to the low reduction efficiency, complexity of the synthesis methods, and limitations in scaling up the catalyst materials. In this work, we have successfully designed and synthesized a series of hollow tubular ZnO@ZnS core-sheath heterostructured materials, by combining radio-frequency thermal plasma and hydrothermal treatment technologies. The S:Zn molar ratio, reaction time, and temperature were systematically investigated, and the morphology of intermediate products was successfully captured, which provided conclusive evidence for the proposed formation mechanism. Notably, the photocatalytic CO yield of the ZS 0.5 O hollow nanotube core-sheath composite is not only 3.20 or 4.03 times higher than that of the pure ZnO or ZnS, respectively, but also possesses excellent stability. By in-depth characterization, we found that the hollow core-sheath heterostructure enhances light capture and absorption, exposes more effective active sites, and builds a type-II heterojunction between ZnO and ZnS to enhance the separation efficiency of charge carriers. The synergy of these factors significantly improves the catalytic performance, offering new insights for photocatalytic, electrocatalytic, and photoelectrocatalytic CO 2 reduction.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Qin Hai-Gang,Du Yun-Fan,Bai Yi-Yang,Li Fu-Zhi,Yue Xian,Wang Hao,Peng Jian-Zhao,Gu Jun
Electrochemical CO 2 reduction in acidic electrolytes is a promising strategy to achieve high utilization efficiency of CO 2 . Although alkali cations in acidic electrolytes play a vital role in suppressing hydrogen evolution and promoting CO 2 reduction, they also cause precipitation of bicarbonate on the gas diffusion electrode (GDE), flooding of electrolyte through the GDE, and drift of the electrolyte pH. In this work, we realize the electroreduction of CO 2 in a metal cation-free acidic electrolyte by covering the catalyst with cross-linked poly-diallyldimethylammonium chloride. This polyelectrolyte provides a high density of cationic sites immobilized on the surface of the catalyst, which suppresses the mass transport of H + and modulates the interfacial field strength. By adopting this strategy, the Faradaic efficiency (FE) of CO reaches 95 ± 3% with the Ag catalyst and the FE of formic acid reaches 76 ± 3% with the In catalyst in a 1.0 pH electrolyte in a flow cell. More importantly, with the metal cation-free acidic electrolyte the amount of electrolyte flooding through the GDE is decreased to 2.5 ± 0.6% of that with alkali cation-containing acidic electrolyte, and the FE of CO maintains above 80% over 36 h of operation at −200 mA·cm −2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Hao Tang,Zi Ang Chen,Muchen Wu,Shunbo Li,Ziran Ye,Mingjia Zhi
Tuning the size of Au nanoparticles is always an interesting task when constructing Au/semiconductor heterojunctions for surface plasmon resonance-enhanced photocatalysis. In particular, the size of Au nanoparticles in the newly emerging “plasmonic aerogel” photocatalyst concept could approach the size of the semiconductor phase. This work provides an alternative route to realize the size tuning of Au nanoparticles in Au-CeO 2 composite aerogels to some extent, within the framework of the well-established epoxide addition sol–gel method. The size tuning is achieved by exploiting the multi-functionalities of a mixed organic acid additive containing a thiol group in the gelation step. The obtained aerogel photocatalysts are composed of a porous backbone of interconnected CeO 2 nanoparticles and Au nanoparticles, and the size of Au nanoparticles ranges from ∼30 nm to sub-10 nm, while the size of CeO 2 remains at ∼15–10 nm. The surface plasmon resonance peak position and intensity contributed by the Au nanoparticles then vary accordingly. Photocatalytic CO 2 reduction at the gas–solid interface is chosen as a model reaction to study the effect of Au nanoparticle size on the photocatalytic activity of composite aerogel photocatalysts. The addition of Au nanoparticles undoubtedly enhances the overall activity of the CeO 2 aerogel photocatalyst, while the degree of enhancement (in terms of total charge consumption) and product selectivity (CH 4 or CO) are different and correlated with the size of the Au nanoparticles. The best performance can be achieved in a composite in which the Au sizes are the smallest.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Qingchun Zhang,Di Liu,Yaping Zhang,Zhiliang Guo,Minpeng Chen,Yuyun Chen,Bo Jin,Yingze Song,Hui Pan
The development of highly active, selective, and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO 2 conversion into fuels or chemicals for mitigating the energy crisis and climate problems. Therefore, it is necessary to achieve the goal through reasonable material design based on the actuality of the operational active site at the molecular scale. Inspired by the stimulating synergistic effect of coupled heteronuclear metal atoms, a novel Ni-Co atomic pairs configuration (denoted as NiN 3 ©CoN 3 -NC) active site was theoretically screened out for improving electrochemical CO 2 reduction reaction (CO 2 RR). The structure of NiN 3 ©CoN 3 -NC was finely regulated by adjusting Zn content in the precursors Zn/Co/Ni-zeolite imidazolate frameworks (Zn/Co/Ni-ZIFs) and pyrolysis temperature. The structural features of NiN 3 ©CoN 3 -NC were systematically confirmed by aberration-corrected HAADF-STEM coupled with 3D atom-overlapping Gaussian-function fitting mapping, XAFS, and XRD. The results of theoretical calculations reveal that the synergistic effect of Ni-Co atomic pairs can effectively promote the *COOH intermediate formation and thus the overall CO 2 RR kinetic was improved, and also restrained the competitive hydrogen evolution reaction. Due to the attributes of Ni-Co atomic pairs configuration, the developed NiN 3 ©CoN 3 -NC with superior catalytic activity, selectivity, and durability, with a high turnover frequency of 2265 h −1 at −1.1 V (vs . RHE) and maximum Faradaic efficiency of 97.7% for CO production. This work demonstrates the great potential of DACs as highly efficient catalysts for CO 2 RR, provides a useful strategy to design heteronuclear DACs, exploits the synergistic effect of multiple metal sites to facilitate complex CO 2 RR catalytic reactions, and inspires more efforts to develop the potential of DACs in various fields.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Xiaohui Wang,Yuanxiangyi Feng,Zhe Li,Jinhua Liu,Dandan Sun,Wei Yang,Xiaowei Xing,Wenjun Liu,Hongxin Zhang
A fluorescent capillary sensor for detecting the bioanalytically and biologically relevant analytes pH, O 2 , and CO 2 has been designed. The sensor is based on single capillary tube with 2 mm inner diameter, which is simultaneous doped with emissive O 2 -sensitive indicator Ru(dpp) 3 (PF6) 2 (RuDP), pH-sensitive and CO 2 -sensitive indicator 8-hydroxypyrene-1, 3,6-trisulfonic acid trisodium salt (HPTS). The multifunctional sensor can be excited at the same wavelength and realize multi-parameter optical monitoring at the different sensing position. Studies in phosphate-buffered solutions display the excellent feasibility of the capillary sensor for fluorescence detection of pH, O 2 , and CO 2 . Overall, the multifunctional capillary sensor exhibits great potential in real-time blood gas analysis, and clinical application of multi-parameter biological detection.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Tete Zhao,Xupeng Zong,Jiuding Liu,Jialei Chen,Keqiang Xu,Xiao Wang,Xijie Chen,Wutong Yang,Fangming Liu,Meng Yu,Fangyi Cheng
Copper-based nanomaterials are attractive in CO 2 electroreduction into valuable chemicals but still suffer from limited selectivity of C 2+ products due to the parasitic hydrogen evolution reaction and inefficient dimerization of absorbed CO intermediate (*CO). Herein, we report an in situ polymerization strategy to coat hydrophobic polymer containing methoxyl silane ((CH 3 O) 3 Si–) and trifluoromethyl (–CF 3 ) functional groups on Cu nanoparticles. The optimized Cu-poly exhibits a high Faradaic efficiency of 71.08 % and a remarkable partial current density of 355.4 mA cm −2 for C 2+ products in a membrane electrode assembly electrolyzer using a bicarbonate electrolyte. A combined study of density functional theory calculations and in situ infrared characterizations indicates that the enhanced performances could be ascribed to the decreased formation energy of *COCOH, induced by the withdraw-electron effect of –CF 3 and enhanced coverage of *CO. This work offers a new insight in tuning the electrocatalytic microenvironment through the surface polymerization process.
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Biomass Conversion and Biorefinery
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2023
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IF 4
Chen Jun Xiu,Li Jin Hao,Bao Agula
The development of porous carbon materials with high CO 2 adsorption capacity is crucial for addressing the current issues of industrial air pollution and global warming. In this study, B/N codoped porous carbon materials were prepared via a combined strategy involving the use of a self-sacrificing template in conjunction with potassium hydroxide activation; moreover, g-C 3 N 4 was used as the N source and boric acid was used as the B source. The pore structure and surface chemistry were investigated in detail using different techniques such as X-ray diffraction, scanning electron microscopy, N 2 adsorption and desorption, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. Results showed that the prepared material exhibited the highest specific surface area (2278 m 2 /g) and pore volume (1.00 cm 3 /g) when the ratio of B/N sources was 1:0.5; moreover, its CO 2 adsorption value (3.26 mmol/g) was higher than those of most codoped adsorbents.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 46
·e54671
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IF 3
Zonglin He,Zhenhong Huang,Jiahui Chen,Ansheng Chen,Jiaoyan Ai,Lina Song,Baohua Liu
Poly (propylene carbonate) diol (PPCD) is one of the most attractive CO 2 copolymers. PPCD-based polyurethane has excellent mechanical properties and hydrophilicity, and is widely used in various fields. However, poor alkali resistance limits the application of PPCD-based polyurethane in wet-type artificial leather (WPL). In order to solve this problem, polyurethane solution (PUS) for wet-type artificial leather was prepared by using PPCD and polytetramethylene ether glycol (PTMG) as soft segments. The chemical structure, viscosity, molecular weight and distribution, physical and mechanical properties, thermal properties and dynamic mechanical thermal properties of PUS were characterized. The changes of the physical and mechanical properties of PUS films and surface morphology of WPLs after soaking in 10 wt% NaOH solution at room temperature for 24 h were studied, so as to evaluate the alkali resistance of polyurethane. The retention of tensile strength and tearing strength of PUS films modified by PTMG increased from 80% to 96% and from 89% to 100%, respectively. The scanning electron microscopy results showed that appropriate PTMG was beneficial to the formation of microporous structure for CO 2 -based polyurethane leather. The leather without PTMG showed agglomeration phenomenon, the micropores were not obvious, and the changes were obvious after soaking in alkali solution. After being modified by PTMG, the morphology of leather after soaking in alkali solution was basically unchanged. Polyurethane leather prepared with PTMG and PPCD as soft segments has excellent alkali resistance. These results suggest that PPCD could be a potential artificial leather material.
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