Nature Communications
·
2025
·Vol. 16
·期 1
·10727
·
IF 15.7
Wang Sifan,Fang Zhecheng,Yu Can,Li Bolong,Wang Jianghao,Zhang Jiaji,Zhang Zihao,Zhou Wenhua,Yao Siyu,Song Weiyu,Liu Zhao-Qing,Cheng Dangguo,Fu Jie
Electrocatalytic reduction of CO 2 to ethylene utilizing Cu-based catalysts in acidic media demonstrates considerable potential for addressing energy and environmental challenges. However, cationic Cu δ+ is apt to be reduced to Cu 0 under the harsh acidic CO 2 reduction conditions. Here we show that the interface of yttrium-doped ZrO 2 and CuO (YSZ/CuO) can stabilize cationic Cu δ+ , preventing its over-reduction even at high applied potentials. The YSZ/CuO catalyst achieves a faradaic efficiency of 68.7% and a partial current density of 545.0 mA·cm –2 for ethylene formation in acidic media (pH = 2). In-situ characterization and theoretical calculations indicate that the abundant oxygen vacancies in YSZ promote the initial formation of interfacial oxygen from CuO rather than the support . The interfacial oxygen derived from CuO offers a high charge density of Cu, facilitated by electron transfer from Zr/Y to Cu, leading to a shortened Cu-O bond and enhances stabilization against reduction. This interface engineering strategy not only protects cationic metals under reducing and acidic conditions but also provides valuable insights applicable across heterogeneous catalysis.
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PubMed
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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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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PubMed
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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
ChemSusChem
·
2019
·Vol. 12
·期 12
·2740-2747
·
IF 7.804
Xiaoli Jin,Chade Lv,Xin Zhou,Liqun Ye,Haiquan Xie,Yue Liu,Huan Su,Biao Zhang,Gang Chen
Graphical Triple boost ! The high abundance of oxygen vacancies in Bi 24 O 31 Cl 10 play the following three roles for fully optimizing the CO 2 conversion efficiency: (i) enhance charge density, (ii) improve separation of electron–hole pairs, and (iii) lower energy for the formation of intermediates during the process. Unearthing an ideal model to describe the role of defect sites for boosting photocatalytic CO 2 reduction is rational and necessary, but it still remains a significant challenge. Herein, oxygen vacancies are introduced on the surface of Bi 24 O 31 Cl 10 photocatalyst (Bi 24 O 31 Cl 10 -OV) for fine-tuning the photocatalytic efficiency. The formation of oxygen vacancies leads to a new donor level near the conduction band minimum, which enables a faster charge transfer and higher carrier density. Moreover, oxygen vacancies can considerably reduce the energy for the formation of COOH* intermediates during CO 2 conversion. As a result, the activity of Bi 24 O 31 Cl 10 -OV for selective photoreduction of CO 2 to CO is significantly improved, with a CO generation rate of 0.9 μmol h −1 g −1 , which is nearly 4 times higher than that of pristine Bi 24 O 31 Cl 10 . This study reinforces our understanding of defect engineering in Bi-based photocatalysts and underscores the potential importance of implanting oxygen vacancies as an effective strategy for solar energy conversion.
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PubMed
高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2016
·Vol. 46
·期 2
·999-1004
·
IF 1.491
Huang Zhengfeng,Cheng Xudong,Dong Peimei,Zhang Xiwen
To mitigate the greenhouse effect, many studies have been carried out to improve the CO 2 conversion efficiency of TiO 2 . Modification of TiO 2 has been intensively investigated, but the influence of an electric field on photoreduction by this material remains largely unknown. Accordingly, in this study, we explored the effect of an electric field on the photoreduction process using a porous TiO 2 -Ti material. The results indicated that the CO yield improved 85-fold (equivalent to 4772 μ mol/g h) when a 30-kV voltage was applied during the reduction process. To make the electric field effect fully functional, we also explored the effect of water on the photoreduction process, finding that TiO 2 showed the highest conversion rate when the humidity was controlled at 50% relative humidity (RH).
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CARBON
·
2019
·
IF 7.466
Yawei Yue,Yangye Sun,Can Tang,Bing Liu,Zhe Ji,Anqi Hu,Bin Shen,Zizhong Zhang,Zhengzong Sun
To reverse the ever-increasing trend of the CO 2 concentration in the atmosphere, human needs to develop a killer “catalyst”, which could convert the anthropogenic CO 2 back into high value-added or energy-storage molecules, not under the natural photosynthesis Calvin cycle, but through an artificial CO 2 reduction pathway. In the race to this emergent technology, the electrochemical reduction of CO 2 (CO 2 RR) with carbon based catalyst becomes one of the frontrunners. However, the carbon-based catalysts are genetically complex, with edge, strain, intrinsic topological defect, and doping effects, coexisting and affecting the catalysis behavior. Without a relative activity ranking system under the same metrics, unveiling the mechanism and improving the catalyst would become formidable. Here we assessed different carbon materials’ CO 2 RR performance under standard experimental conditions. The catalytic activities were evaluated and sequenced by their cathodic potential, characterized with the peak CO faradic efficiency . The doping effect is leading in the sequence, followed with the other three factors, all of which are superior to the pristine sp 2 carbon material.
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高影响因子
ACS Applied Nano Materials
·
2020
·
IF 0
Siyu Kuang,Minglu Li,Rong Xia,Lei Xing,Yaqiong Su,Qun Fan,Jinping Liu,Emiel J.M. Hensen,Xinbin Ma,Sheng Zhang
The electrochemical carbon dioxide reduction reaction (CO2RR) is a promising solution to the current environmental and energy issues. Cu is the only metal catalyst able to convert CO2 into high-value-added hydrocarbons. However, Cu catalysts tend to degrade with the decrease in the hydrocarbon selectivity under operation conditions. Herein, we monitored the morphological evolution of Cu nanocatalysts and correlated with changes in the selectivity of hydrocarbon products during electrochemical CO2 reduction. Initial Cu nanospheres quickly reconstructed into nanocubes within 1 h of CO2 electrolysis and then gradually turned into even smaller irregular nanoparticles. Interestingly, the above unstable Cu nanocube offered the maximum ethylene selectivity. We successfully stabilized these Cu nanocubes using a 2D graphene surface doped with nitrogen to achieve high ethylene selectivity over 24 h. Our X-ray photoelectron spectroscopy (XPS) and density-functional theory (DFT) investigations show that the strong interaction between Cu and pyridinic nitrogen on the 2D graphene surface plays a key role in stabilizing Cu nanocubes.
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