Advanced Energy Materials
·
2025
·
IF 26
Ruizhe Yang,Lu Xia,Wulyu Jiang,Yi Cheng,Kaiwen Wang,Tengyu Chen,Fei Li,Xiaoli Zhao,Bin Wang,Yingtang Zhou,F. Pelayo García de Arquer,Ming Huang
Carbon dioxide electroreduction reaction (CO 2 RR) offers a pathway to convert CO 2 into valuable multicarbon products (C 2+ ), potential clean energy, and chemical vectors, using renewable electricity. Copper catalysts are, so far, the most selective in this process, but still face challenges such as high overpotentials and insufficient selectivity and stability when used alone. One strategy to tackle these is the use of Cu-based tandem structures, which incorporate tailored reaction sites to drive a segment of the CO 2 RR reaction, in a more favorable way, within the same electrode. Recent examples have shown how Cu-tandem catalysts can lead to voltage savings and improvements in selectivity. This review analyses various Cu-based tandem catalysts, focusing on alloys, heterostructures (especially highlighting the role of polymer coatings in achieving tandem effects through environmental control), and metal–organic frameworks (MOFs). It covers synthetic strategies to achieve tandem-enabling configurations and their suggested impact on reaction mechanisms and performance improvement toward C 2+ electrosynthesis. The review concludes by offering a roadmap toward the design of more efficient Cu-based tandem electrodes for CO₂RR and beyond.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Sheng Chang,Yimin Xuan,Jingjing Duan,Kai Zhang
Electrochemical CO 2 conversion into valuable products provides a promising solution for achieving a carbon-neutral energy cycle. Herein, an active and stable Bi/Nafion interface is fabricated over Bi nanosheets with the modification of Nafion, which exhibits superior CO 2 conversion with formate selectivity of above 95% in a wide potential range, partial current density of 72.12 mA cm −2 at − 1.07 V vs. RHE in H-type cell. The extraordinary CO 2 reduction performance could be ascribed to a high CO 2 permeability and enhanced local proton activity at the Bi/Nafion interface, which leads to promoted CO 2 adsorption and feasible proton-coupled electron transfer during the CO 2 reduction process. Computational investigations reveal the modification of Nafion offers a comfortable platform to enable the key intermediate *OCHO to be stable. This work offers a valuable insight into interfacial manipulation of electrodes to convert CO 2 to valuable products.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Xiaofan Yang,Siyu Yi,Zhaolong Wang,Zhongqiu Wu,Ying Zhang,Junjie Yuan,Haibo Wang,Xiaojie She,Hui Xu
Electrocatalytic CO2 Reduction Reaction (ECO2RR) driven by renewable energy, which could convert CO2 into fuels or value-added chemicals, has become an effective approach to address environmental issues and the energy crisis. However, due to the low selectivity, the inferior activity, and unmanageable reconstruction of catalysts, the path of ECO2RR remains a significant challenge. In this study, a series of electrocatalysts composed of copper–lanthanum nanoparticles dispersed within a nitrogen-doped carbon framework (LaCu@NCF-x, where x represents the abbreviation of calcination temperatures) were synthesized by calcining the mixture of polymers and metal ions, in which thermal control is the key to the catalyst preparation process. Phase and morphological characterizations reveal that the degree of carbonization and the accessibility of active sites were modulated by the temperature of calcination. The study highlights the importance of the synergistic and confinement effects of the encapsulating carbon layer, which not only provides a favorable matrix for the nanoparticles but also mitigates the reconstruction of electrocatalysts, thereby significantly enhancing its performance in CH4 production during ECO2RR. In particular, the LaCu@NCF-3 catalyst demonstrates the maximum Faraday efficiency (FE) of CH4 up to 64.6% at −1.177 V vs RHE and superior stability. Moreover, it also maintains a high selectivity (FECH4 ≥ 60%) over the wide potential range from −0.977 V to −1.577 V vs RHE. This study provides a novel approach to the fabrication of efficient and stable Cu-based electrocatalyst for ECO2RR to CH4.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Qinghua Qu,Yuqiao Jiang,Linyan Cheng,Qingyuan Xue,Ranran Li,Cheng Fang,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan
Covalent organic frameworks (COFs) with high specific surface area, ordered pore wall, modified porous surface and customizable chemical structure have been widely used in CO 2 capture. However, the screening of functionalized COFs suitable for CO 2 capture still relies on experiments, which will require a long experimental period with blindness and randomness. Herein, we chosed three electron withdrawing groups (–NO 2 , –CN and −Br) and three electron donating groups (–CH 2 NH 2 , –CH 3 , –OCH 3 ) to explore the effect of electron withdrawing ability of functional groups on the CO 2 adsorption capacity. Grand canonical Monte Carlo (GCMC) method was used to simulate the adsorption capacity of CO 2 over X-TpBD-COFs (X=–NO 2 , –CN, −Br, –CH 2 NH 2 , –CH 3 , –OCH 3 ). As the result, NO 2 -TpBD-COF had the highest adsorption capacity among the six functionalized X-TpBD-COFs at 100 kPa and 25 ℃ (49.37 cm 3 /g), while OCH 3 -TpBD-COF had the lowest adsorption capacity among them (23.51 cm 3 /g at 25 ℃ and 100 kPa). The order of binding energy was basically the same as the order of adsorption capacity when the synergistic interactions between functional groups and oxygen atoms in Tp were considered according to density functional theory (DFT). Molecular dynamics (MD) showed that the diffusion and distribution of CO 2 were mainly effected by pore structures. To verify the simulation results, NO 2 -TpBD-COF and OCH 3 -TpBD-COF were successfully prepared by solvothermal method. The CO 2 adsorption capacities of these two COFs were basically consistent with the conclusion obtained by the simulations. This study provided a way for simulation to guide accurate and rapid experimental design of COF materials for CO 2 capture.
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DOI
高影响因子
Journal of CO2 Utilization
·
2024
·
IF 7.2
Xiaomeng Deng,Wensheng Wei,Zizhen Yan,Zhanguo Zhang,Yuxin Wang,Guangwen Xu,Jianjun Guo,Jinggang Zhao,Lei Shi
A meaningful and practical phenomenon was observed and investigated, about which a synthesized (2-hydroxyethyl) triethylammonium bromide (NEt 3 (HE)Br) was used for catalytic cycloaddition of PO (propylene oxide) and CO 2 (carbon dioxide) in a homogeneous state, and then separated from the reaction system in a heterogeneous state. The target products were first reported as additives to regulate the distribution of reactants and carbon dioxide (CO 2 ) in the gas-liquid phase, as well as to facilitate the dissolution of NEt 3 (HE)Br. Under the optimal conditions of 0.2 mol% NEt 3 (HE)Br dosage, the PC yield (98.71 %) and TOF value (22.54 h −1 ) reached are significantly higher than the case of without PC addition. Besides, NEt 3 (HE)Br exhibited impressive stability after five catalytic cycles. The catalytic performances of different additives (i.e., alcohols, cyclic carbonate, amides, sulfones, petroleum ether, straight-chain carbonate and oxalate) were investigated, and their promotional effects and mechanisms were systematically elucidated. The transition behavior of dissolution-catalysis-precipitation process and intrinsic promoting mechanism of NEt 3 (HE)Br gave an efficient idea for a homogeneous catalytic reaction and heterogeneous separation of the catalyst. Meanwhile, this work provides an important theoretical and practical basis for efficient and facile catalyst synthesis and the corresponding reaction system design.
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高影响因子
Frontiers in Chemistry
·
2020
·
IF 3.693
Lai Nanjun,Zhu Qingru,Qiao Dongyu,Chen Ke,Tang Lei,Wang Dongdong,He Wei,Chen Yuemei,Yu Tong
To improve CO2 adsorption performance of nanoparticle absorbents, a novel tertiary amine functionalized nano–SiO2 (NS–NR2) was synthesized based on the 3–aminopropyltrimethoxysilane (KH540) modified nano–SiO2 (NS–NH2) via methylation. The chemical structure and performances of the NS–NR2 were characterized through a series of experiments, which revealed that NS–NR2 can react with CO2 in water and nanofluid with low viscosity revealed better CO2 capture. The CO2 capture mechanism of NS–NR2 was studied by kinetic models. From the correlation coefficient, the pseudo second order model was found to fit well with the experiment data. The influencing factors were investigated, including temperature, dispersants, and cycling numbers. Results has shown the additional surfactant to greatly promote the CO2 adsorption performance of NS–NR2 because of the better dispersity of nanoparticles. This work proved that NS–NR2 yields low viscosity, high capacity for CO2 capture, and good regenerability in water. NS–NR2 with high CO2 capture will play a role in storing CO2 to enhanced oil recovery in CO2 flooding.
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DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 6
·期 3
·2252-2258
·
IF 3.84
Yun Qin,Jianfei Lv,Xin Fu,Ruili Guo,Xueqin Li,Jianshu Zhang,Zhong Wei
Three types of amino acid salts (sodium lysine, sodium arginine, sodium histidine) were introduced into SPEEK polymer matrix to fabricate a series of SPEEK/amino acid salt membranes for CO2 separation. The membranes could efficiently separate CO2 from a CO2/CH4 mixture due to the simultaneous improvement of CO2 permeability and separation performance. Firstly, the amino acid salt contained a larger number of amino groups (–NH2), which could reversibly react with CO2, improving the CO2 molecules transfer performance. Secondly, the ether oxygen structure (–O–) in the polymer chain and the carboxyl groups (–COO−) in the amino acid salt had an excellent affinity for CO2, enhancing the solubility selectivity. Thirdly, the introduction of amino acid salt increased the water uptake, and water was favored over CO2 dissolution; this was also good for the increase of solubility selectivity. Among the three types of amino acid salts, the membrane doped with 20 wt% sodium lysine (SPEEK/LLS-20) showed the highest CO2 permeability of 295.6 barrer and CO2/CH4 selectivity of 71.8 at 2 bar and room temperature, surpassing the 2008 Robeson upper bound line.
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LANGMUIR
·
2019
·
IF 3.683
Xiaojiang Li,Baogang Wang,Shanshan Dai,Hongsheng Lu,Zhiyu Huang
CO2-responsive microemulsions based on ionic liquid 1,1,3,3-tetramethylguanidine-oleic acid (TMG-OA) have been designed to provide an approach for reducing the volatilization of amine in amine-containing microemulsions effectively and exhibit reversible transitions of microstructures. The ionic liquid TMG-OA was prepared by the direct neutralization of oleic acid (HOA) and 1,1,3,3-tetramethylguanidine (TMG, one of volatile and toxic amines). From the investigations of nuclear magnetic resonance hydrogen spectrum, pH, thermogravimetry, and automatic interface tension meter, the excellent properties of switchability, stability, and surface activity of TMG-OA were demonstrated, and then the ionic liquid-based microemulsions with CO2 response were prepared with TMG-OA (surfactant), HOA (oil phase), isopropyl alcohol (IPA, cosurfactant), and water. Interestingly, for microemulsions with a higher IPA content (47.42, 44.48 wt %), sizes of microemulsions are increased upon introducing CO2 and decreased upon addition of N2/65 °C. In addition, for microemulsions with a lower IPA content (26.22 wt %), the new microemulsions with different sizes are regenerated after the phase separation of emulsions generated by introducing CO2, and incomplete recovery of microemulsions can be observed upon addition of N2/65 °C. The reversible microstructures are induced by the swelling behavior and the reduced single phase area, which are caused by the reversible conversion between TMG-OA and HOA components.
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DOI
PubMed
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Lei Xiong,Xianbiao Fu,Yu Zhou,Pei Nian,Zheng Wang,Qin Yue
Electrochemical CO2-to-CO conversion is a significant alternative to lower CO2 emission and build carbon-neutral processes, as well as produce CO, which can directly serve as a syngas precursor for Fischer–Tropsch synthesis. However, the easy water flooding of the gas diffusion electrode (GDE) employed in a flow cell during CO2 reduction reaction (CO2RR) electrolysis remains a tough problem. Consequently, it breaks the electrolyte/catalyst/CO2 triphase interface and lowers the FECO. Herein, the combined inarching of amino-substituted cobalt phthalocyanine (CoPc-NH2) and octadecylamine (ODA) onto the surface of the CNT via an amide bond was designed and fabricated. The obtained composite catalyst, labeled as CoPc-CNT-ODA, shows atomically dispersed metal active sites endowed with superior and stable hydrophobicity. When applied to CO2RR in a flow cell, the CoPc-CNT-ODA electrode displays a high CO faradic efficiency (FECO) of 97.7% and a partial current density (jCO) of 154.8 mA·cm–2 at an applied potential of −1.0 V (vs RHE). Moreover, the FECO values are all above 90% from −0.8 to −1.2 V (vs RHE). Even after electrolyzing at −1.0 V for 12 h, the FECO still remains at 88.3%, implying the superior stability of the CoPc-CNT-ODA electrode. The proposed methodology for GDE/catalyst improvement can be extended to other triphase interfaces involved in catalytic systems.
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高影响因子
JOURNAL OF CHEMICAL ENGINEERING OF JAPAN
·
2015
·Vol. 48
·期 4
·268-275
·
IF 0.644
Da-Niu Cai,Kuan Huang,Xiao-Min Zhang,Xing-Bang Hu,You-Ting Wu
Amino acids were used to modify macroreticular ion exchange resin for the adsorptive capture of CO2. Adsorption isotherms, adsorption rate curves, heats of adsorption, and gas separation performance were determined. It is found that the adsorption capacity of the resin increases significantly after the loading of amino acids. The adsorption progresses rapidly and reaches equilibrium within 3 min. The adsorption capacity decreases with the increasing temperature, and room temperature is a suitable condition that enables high adsorption of CO2. The adsorbent can be promoted by water vapor in removing CO2 effectively from gas mixtures. Ten continuous adsorption–desorption cycles was performed, showing that the adsorbent is of good regeneration performance and the adsorption capacity keeps at about 0.9 mmol/g after regeneration.
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高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2016
·Vol. 32
·期 3
·605-610
·
IF 0.844
CHEN Feng-Feng,DONG Yan,SANG Xiao-Yan,ZHOU Yan,TAO Duan-Jian
Four tetrabutylphosphonium carboxylate ionic liquids ([P4444][CA]) were prepared, and their densities, viscosities, refractive indices, and conductivities were measured and correlated with thermodynamic and empirical equations in the temperature range of 298.15-348.15 K.
The influence of temperature on these four properties of [P4444][CA] was discussed, and their thermal expansion coefficient values were calculated. The CO2 absorption capacity of [P4444][CA] was studied at 313.15 K and 100 kPa. The results indicated that [P4444][Buty]
had the highest CO2 capture capacity among these ionic liquids, with an absorption capacity of 0.4 mol·mol-1 and balance time of less than 5 min.
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ADSORPTION SCIENCE & TECHNOLOGY
·
2013
·
IF 0.559
Jiaodi Tang,Yaping Zhou,Wei Su,Xiuwu Liu,Yan Sun
Zeolite SSZ-13 was synthesized by a traditional hydrothermal method, and characterized by powder X-ray diffraction, scanning electron microscopy and transmission electron microscopy. The porous structure of the samples was determined from nitrogen uptake measurements at 77 K, and the surface properties were analyzed by Fourier transform infrared spectroscopy. The zeolite SSZ-13 had a type I isotherm with a uniform pore-size distribution and most pores were less than 1 nm. The Langmuir surface area was 703 m2/g. The adsorption of various gases on SSZ-13 was studied experimentally and a high selectivity for CO2 over N2 was achieved.
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高影响因子
危险品化学品经营许可证（带存储）