Chem Catalysis
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2022
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IF 0
Wenjie Wu,Yulu Yang,Yitong Wang,Tiantian Lu,Qingsong Dong,Junwei Zhao,Jingyang Niu,Qingchao Liu,Zhaomin Hao,Shuyan Song
Electrosynthesis of urea from N 2 and CO 2 molecules is of immense significance but has so far been plagued by the lack of a universal design principle to guide the search for new catalysts. Herein, as exemplified by the Cu-Bi catalyst, our findings revealed that the defective Cu-Bi catalyst could offer a maximum urea concentration of 0.45 ± 0.06 mg L −1 and the largest faradaic efficiency of 8.7% ± 1.7% at −0.4 V (versus reversible hydrogen electrode [RHE]), exhibiting outstanding activity in contrast to monometallic (Cu and Bi) and bimetallic (Cu-Bi mixture and intact Cu-Bi) catalysts. Moreover, the evidence from isotope tracing experiments, in situ Raman spectroscopy, and density functional theory (DFT) calculations suggested that it is a promising strategy for the co-reduction of N 2 and CO 2 by defective Cu-Bi catalysts, switching on a light to the application of defects in electrosynthesis of urea.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xinyi Wan,Ting Wan,Chaochao Cao,Chengchun Tang,Yanming Xue,Youguo Yan,Zhen Li,Zhizhen Ye,Xinsheng Peng
The development of highly effective and durable CO 2 separation membrane is still a challenge for the carbon capture and storage. Herein, a novel BN nanosheets supported magnetic ionic liquid membrane (BN-SMILM) is constructed by nanoconfining magnetic ionic liquid (MIL) [P 6,6,6,14 ][FeCl 4 ] to the two-dimentional (2D) nanochannels of laminated BN membrane. The 2D nanochannels provide a well support and restricted space for the MIL. The nanoconfinement effect makes the magnetic [FeCl 4 ] - anions align along the center of 2D BN nanochannels, leading to selectively accelerate the CO 2 transport. The nanoconfinement effect and CO 2 separation mechanism are further explicated by the molecular dynamic simulations. As a result, compared with the polymer supported MIL membrane, the as-prepared BN-SMILM exhibits better CO 2 separation performance, with CO 2 permeability of about 227 Barrer and CO 2 /N 2 selectivity of 90 that is above the 2008 Robeson upper-bound. The BN-SMILM also presents excellent long-term stability after 7 days operation, revealing the promising applications in CO 2 separation. This work provides a new strategy to prepare high-performance supported liquid membrane materials towards practical environmental and energy application.
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Nature Communications
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2020
·Vol. 11
·期 1
·1-9
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IF 12.121
Wang Lingxiang,Guan Erjia,Wang Yeqing,Wang Liang,Gong Zhongmiao,Cui Yi,Meng Xiangju,Gates Bruce C.,Xiao Feng-Shou
The reaction pathways on supported catalysts can be tuned by optimizing the catalyst structures, which helps the development of efficient catalysts. Such design is particularly desired for CO 2 hydrogenation, which is characterized by complex pathways and multiple products. Here, we report an investigation of supported cobalt, which is known for its hydrocarbon production and ability to turn into a selective catalyst for methanol synthesis in CO 2 hydrogenation which exhibits good activity and stability. The crucial technique is to use the silica, acting as a support and ligand, to modify the cobalt species via Co‒O‒SiO n linkages, which favor the reactivity of spectroscopically identified *CH 3 O intermediates, that more readily undergo hydrogenation to methanol than the C‒O dissociation associated with hydrocarbon formation. Cobalt catalysts in this class offer appealing opportunities for optimizing selectivity in CO 2 hydrogenation and producing high-grade methanol. By identifying this function of silica, we provide support for rationally controlling these reaction pathways.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
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IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
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Journal of Nano Research
·
2023
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IF 1.7
Yong Qiang Dang,Xiang Yu Feng,Bo Ni Li,Rui Huang,Jia Jia,Jian Lan Zhang,Ya Ting Zhang
Photocatalytic CO2 reduction to solar fuel is a potential way to overcome the problem of high carbon dioxide concentrations; however, the process still faces enormous challenges, such as the low light absorption efficiency and high carrier recombination rates. This work synthesized tetraphenylporphyrin-based carbon dots (TPP-CDs) for the photocatalytic CO2 reduction to CH3OH under simulated sunlight to extend the absorption region of the CDs. The conduction band of the TPP-CDs has a sufficiently negative reduction potential to reduce CO2. TPP-CDs containing 1 wt.% TPP achieved an optimum CH3OH production rate of 173.35 μmol·gcat-1·h-1, with a remarkable 2.06-fold increase compared to pristine CDs without TPP. In this study, TPP-CDs were synthesized by changing the CD precursors to improve the utilization of visible light and apply them to the photocatalytic reduction of CO2.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Yulin Tan,Ziye Shen,Ying Yang,Huimin Zhang,Yufang Xie,Chenglin Zhang,Yuan Liu,Mingming Chen,Dawei Cao
Heterojunction engineering significantly enhances photocatalytic CO 2 reduction performance. However, a large lattice mismatch in heterostructures hinders photocatalytic reaction by forming extensive grain boundaries, inefficient interfaces, and sluggish interfacial charge transfer. Metal halide perovskites, featuring soft lattices induced by weak ionic metal-halide bonds, offer effective solutions to alleviate such mismatches. Herein, we fabricate BaTiO 3 /CsPbBr 3 photocatalysts with a precisely engineered type-II heterojunction. Notably, the BaTiO 3 /CsPbBr 3 heterostructure achieves a CO formation rate of 17.3 μmol∙g −1 h −1 — 5.2-fold and 2.3-fold higher than pristine BaTiO 3 (3.3 μmol∙g −1 h −1 ) and CsPbBr 3 (7.6 μmol∙g −1 h −1 ), respectively. This improvement stems from the synergistic effect of enhanced light absorption and charge separation. This work provides fundamental insights for developing high-performance heterojunction photocatalysts.
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高影响因子
Nature Communications
·
2025
·
IF 15.7
Ren Yuqi,Cheng Miao,He Hongbin,You Changjun,Duan Lunbo,Sun Zhenkun,Peng Ruoxuan,Zhu Yuan-Hao,Zhang Hongyang,Zhou Jiancheng,Huang Kai,Guan Jie,Li Naixu
CO 2 -to-hydrocarbon fuel conversion via artificial photosynthesis is limited by catalyst poisoning under high O 2 partial pressures and sluggish C 2 -product formation. Herein, Ru 0.6 Cu 1 (Cu 0 –Cu 1+ )/CeO 2 catalysts with adaptive O 2 tolerance are prepared by O 2 -mediated dynamic interfacial reconstruction. Single-atom Ru doping at Ce lattice sites creates a trigonal prismatic coordination configuration, enabling proton-coupled electron transfer and accelerating H 2 O dissociation. Photothermal effect promotes O 2 -driven self-assembly of Cu 0 –Cu 1+ charge-gradient interfaces within Ru/Cu alloy clusters, thereby optimizing the adsorption behavior of * CHOCO intermediates and restructuring the C–C coupling pathway. Interfacial charge cascade transfer and geometric site synergy thermodynamically shift the product selectivity from C 1 to C 2 , as determined by operando spectroscopy and electronic structure analysis. Under concentrated solar irradiation, the catalyst produces 549 ± 20 μmol·g −1 C 2 H 4 with 74.3% selectivity and 0.5% solar-to-chemical energy conversion efficiency—25-fold higher than that in non-concentrated systems. Dynamic interfacial regulation facilitates precise carbon chain synthesis in complex reaction networks.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jiangtao Peng,Xuanrong Wang,Ming Wen,Shengjie Jiu,Xia An,Xu Wu
The clay mineral-based composite was explored for adsorption of CO 2 , which was fabricated by impregnating monoethanolamine (MEA) on montmorillonite (Mont). The hydroxyl groups of Mont removed, and was found to be only physical loaded-amines after thermal treatment (T-Mont). The MEA molecules were well combined with the -OH surface of Mont, which enhanced stability and cyclability for CO 2 adsorption. The composite 40-MEA@Mont displayed excellent adsorption performance, and adsorption capacity reached 8.72 cm 3 ∙g −1 at room temperature. After eight cycles of CO 2 adsorption, the capacity of 40-MEA@Mont showed no noticeable changes compared to the first cycle, whereas 40-MEA@T-Mont was 15.19 % decline. The reason lies in the hydrogen bond interaction between amine and Mont matrix which was further confirmed by DFT calculation. Isosteric heat of adsorption analysis and in situ FT-IR manifested that CO 2 adsorption predominantly involved weak chemisorption on the composite 40-MEA@Mont. The CO 2 adsorption mechanisms of clay-based support can be controlled by adjusting the type of impregnated amines, and the layered montmorillonite loaded with amines can be a promising material for CO 2 adsorption at room temperature.
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高影响因子
Journal of Cleaner Production
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2025
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IF 10
Jubao Gao,Jinyu Bai,Lu Jia,Xueyi Song,Shujuan Wang,Yongqiang Ren,Shisen Xu
Global climate catastrophes driven by the greenhouse effect and rising CO 2 emissions highlight the urgent need for improved carbon-capture technologies. Deep eutectic solvents (DESs) have emerged as promising alternatives to ionic liquids and aqueous amines, but few studies assess the energy consumption of CO 2 capture with ternary DESs. The present study synthesized novel ternary DESs using cyclic amines as promoters, which were selected on the basis of their stability, slower consumption, and easier bond cleavage. The CO 2 capture performance of the resulting DESs was then investigated using spectroscopy and molecular dynamics simulations. The DES [ChCl][MEA]-5 %PZ exhibited the highest absorption capacity (0.290 g CO 2 /g), representing a 146 % increase over 30 wt % MEA, and an estimated regeneration efficiency of 88 %. Simulations showed that secondary amines strengthen intermolecular interactions and promote CO 2 uptake, consistent with experimental results. The results of both nuclear magnetic resonance and Fourier-transform infrared spectroscopy analyses indicate that CO 2 reacts with cyclic secondary amines to form carbamates, which enhance capture capacity. The heat of reaction was identified as the main contributor to regeneration energy. It is noteworthy that the regeneration energy for [ChCl][MEA]-5 %IM was 1.79 GJ/t CO 2 , which is approximately 60 % of that for 30 wt % MEA and is comparable to biphasic absorbents. In conclusion, these ternary DESs demonstrate considerable potential for energy-efficient CO 2 capture.
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高影响因子
LANGMUIR
·
2025
·
IF 3.9
Weiqiao Zhong,Zhichao Xia,Tingxi Zhang,Yuhuan Nie,Rong Lei,Lu Li,Qibin Chen
Switchable surfactants are an emerging class of environmentally friendly compounds that can be reversibly triggered between active and inactive states in response to external stimuli, enabling on-demand or on-command control over the interfacial properties. In this work, a type of imidazoline-based CO2-switchable surfactants was synthesized and systematically investigated. Structural characterization was performed by using Fourier transform infrared and 1H NMR spectroscopy, confirming the successful formation of long-chain alkyl imidazolines. Their surface activity and critical micelle concentration (CMC) were evaluated by measuring surface tension and interfacial tension, revealing strong adsorption behavior and efficient micellization. Conductivity and NMR analyses demonstrated the reversible transition between neutral and ionic forms under alternating CO2/N2 bubbling, confirming the robustness and repeatability of the switching process. The emulsification/demulsification cycles were repeated over multiple switching operations, where oil/water emulsions were stabilized by their bicarbonate salt forms with long-term stability, whereas the neutral forms induced rapid demulsification. These findings not only establish the fundamental interfacial behavior of imidazoline-based surfactants but also highlight their potential applications in enhanced oil recovery, chemical separation, drug delivery, and sustainable process design.
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PubMed
高影响因子
Science China-Chemistry
·
2020
·Vol. 63
·期 12
·1727-1733
·
IF 6.356
Ren Xinyi,Liu Song,Li Huicong,Ding Jie,Liu Linghui,Kuang Zhichong,Li Ling,Yang Hongbin,Bai Fuquan,Huang Yanqiang,Zhang Tao,Liu Bin
Electrochemical carbon dioxide reduction reaction (CO 2 RR) powered by renewable electricity offers an attractive approach to reduce carbon emission and at the same time produce valuable chemicals/fuels. To design efficient CO 2 reduction electrocatalyst, it is important to understand the structure-activity relationship. Herein, we design a series of single Co atoms electrocatalysts with well-defined active sites electronic structures, which exhibit outstanding CO 2 RR activity with controllable selectivity to CO. Experimental and density functional theory (DFT) calculation studies show that introducing nitro (amino) ligand next to single Co atom catalytic center with electron-withdrawing (electron-donating) capability favors (hinders) CO 2 reduction catalysis. This work provides an in-depth understanding of how functional ligand affects the splitting of transition metal 3d electron orbital, thereby changing the electron transfer from transition metal active site to CO 2 , which is closely related to the Gibbs free energy of the rate-determining step (CO 2 +e − +*→*CO 2 − ).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Wenjian Yue,Zhiyu Huang,Mengli Xiao,Xiaojiang Li,Wenjing Ma,Ying Zhang,Shanshan Dai,Hongsheng Lu
In this article, a higher fatty acid-based ternary CO2-controllable dual-circulation had been successfully constructed, where it provided an excellent oil recovery performance and all solvents could be cycled. This dual-circulation adopted the oil-soluble higher fatty acid (HFA) as the outside loop to extract oil and selected poly(propylene glycol) bis(2-aminopropylether) (Jeffamine D230) as the inner loop to impel the outside loop. In washing oil technology, D230 and HFA as cleaning solvents are ideal substitutes for traditional tertiary amines. First, there is the electrostatic interaction between HFA (represented by n-decanoic acid) and D230, as detected by 1H MNR. The circulation of the system is supported by the rapid CO2-switchable behaviors of HFA-D230, where the reversible phenomenon was recorded by a pH meter and a conductivity meter. In addition, the HFA/D230/water system has demonstrated the cyclic process of dissolving the oil in the simulated oil (the dodecane, kerosene, and diesel) recovery experiment. Finally, the n-decanoic acid (C10-HFA)/D230/water ternary dual-circulation system was obtained as the optimal scheme due to its excellent recovery and separation property. During the separation of simulated oil by using the C10-HFA/D230/water system, the recovery rate of the simulated oil was more than 93% and there was no residual n-decanoic acid by GC/MS analysis. This dual-circulation was successfully established, providing a new method to replace the traditional tertiary amine for oil recovery.
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