APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Shujin Shen,Cheng Han,Bing Wang,Yiang Du,Yingde Wang
Electroreduction of aqueous CO 2 is a sustainable approach to produce tunable syngas, which demands the rational design of dual-active-sites catalysts for individual CO 2 reduction reaction (CRR) and hydrogen evolution reaction (HER). Here, the self-supporting nickel@nitrogen-doped carbon nanotubes grown on carbon nanofiber (Ni@NCNTs-CNF) is developed with Ni single atoms (SAs) and nanoparticles (NPs) functioning as CRR and HER sites respectively. Benefiting from the hierarchical nanostructures for effective electron transport and mass diffusion, as well as the high accessibility of dual-active sites, Ni@NCNTs-CNF catalysts can mediate aqueous CO 2 into CO/H 2 (2:1) with a 100 % Faraday efficiency and a high current density (25 mA cm −2 ) at low working potential (-0.8 V). By manipulating the Ni SAs/Ni NPs ratio, the CO/H 2 proportion is easily modulated in a wide range from 1:4 to 5:1, independence of the working potential (-0.6 to -0.8 V). Our findings provide fresh insights into the design of dual-active-sites catalysts.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 32
·13755-13763
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IF 3.288
Xia Wang,Wulan Zeng,Wenjing Liu,Xiaoyu Cao,Chunhui Hou,Qi Ding,Yaxuan Lü
The design and development of low-cost sorbents is vital for CO2 capture from flue gases. In this study, the lignite char from Ordos coal (SE) was treated by a one-step KOH activation method to prepare microporous activated carbons for CO2 adsorption. The textural pore properties, surface functional groups and element contents of SE before and after activation were characterized and discussed; the effects of the mass ratio of KOH to SE, activation temperature and time, as well as the adsorption temperature on CO2 adsorption for prepared porous sorbents were investigated and optimized; the isosteric heat of adsorption and adsorption kinetics for the optimized sorbent were further calculated and fitted. When the mass ratio of KOH to SE was 1 : 1, the activation temperature and time were 700 °C and 120 min respectively, and the sorbent of K/SE700(120) showed an adsorption capacity of 1.35 mmol g−1 at 20 °C, which dropped by 2.96% after ten regenerations. The Langmuir adsorption isotherms fitted the adsorption data of K/SE700(120) well, and the isosteric heats of adsorption were 11–13 kJ mol−1, showing the physisorption characteristic. In addition, the good fit of the adsorption data to the Avrami model suggested that there are multiple adsorption routes for K/SE700(120).
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CHINESE JOURNAL OF CATALYSIS
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2019
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IF 4.914
Ziyan Zhao,Dmitry E. Doronkin,Yinghao Ye,Jan-Dierk Grunwaldt,Zeai Huang,Ying Zhou
Light illumination has been widely used to promote activity and selectivity of traditional thermal catalysts. Nevertheless, the role of light irradiation during catalytic reactions is not well understood. In this work, Pt/Al 2 O 3 prepared by wet impregnation was used for photothermal CO 2 hydrogenation, and it showed a photothermal effect. Hence, operando diffuse reflectance infrared Fourier-transform spectroscopy and density functional theory calculations were conducted on Pt/Al 2 O 3 to gain insights into the reaction mechanism. The results indicated that CO desorption from Pt sites including step sites (Pt step ) or/and terrace site (Pt terrace ) is an important step during CO 2 hydrogenation to free the active Pt sites. Notably, visible light illumination and temperature affected the CO desorption in different ways. The calculated adsorption energy of CO on Pt step and Pt terrace sites was −1.24 and −1.43 eV, respectively. Hence, CO is more strongly bound to the Pt step sites. During heating in the dark, CO preferentially desorbs from the Pt terrace site. However, the additional light irradiation facilitates transfer of CO from the Pt step to Pt terrace sites and its subsequent desorption from the Pt terrace sites, thus promoting the CO 2 hydrogenation.
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Sustainable Energy & Fuels
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2019
·Vol. 4
·期 3
·1191-1198
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IF 4.912
Zhen Wang,Yiming Zhang,Jing Wang,Yatao Zhang
Carbonic anhydrase (CA) shows a strong affinity for CO2 and is, therefore, widely used in separation membranes for CO2 capture. Herein, a novel biomimetic material (Co-BBP) that can mimic the active site of CA was successfully synthesized and loaded on the surface of porous organic polymers (POPs). Mixed matrix membranes (MMMs) were then manufactured by incorporating Co-BBP@POP-1 nano-composites into the Pebax matrix to improve the CO2 separation performance. Compared with the MMMs doped with Co-BBP or POP-1, the prepared MMMs doped with Co-BBP@POP-1 showed exceptional CO2 separation performance owing to their synergistic effect. The MMMs containing 5 wt% of Co-BBP@POP-1 showed the optimum state with CO2 permeability of 886 Barrer and CO2/N2 selectivity of 94.2, which surpassed the Robeson upper bound (2008). Compared with the observations for the pristine Pebax membrane, the CO2 permeability and CO2/N2 selectivity of MMMs increased by 9.5 times and 3 times, respectively. In short, the combination of Co-BBP and POP-1 provides a good method for the application of biomimetic enzymes and may expand the synergistic effect strategy for preparing biomimetic membranes for CO2 capture.
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JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
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2019
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IF 2.886
Qingfeng Hou,Yuanyuan Wang,Zhe Wang,Qi Wu,Fan Wang,Chen Ni,Xiaobo Zheng,Yan Xu,Yujun Zhao
In this study, a series of CO 2 -switchable acetamidines surfactants with different hydrophobic tail groups were synthesized using N, N-dimethylacetamide dimethyl acetal and different aliphatic amines. The conductivity assessment demonstrated the exceptional CO 2 -switchable performance of these surfactants. It was believed this switchability mainly resulted from the activity of acetamidine groups which could react with CO 2 to form the amphiphilic acetamidine carbonate. For this reason, the protonation during CO 2 bubbling of acetamidine surfactants with longer hydrophobic tail was more likely to occur at higher temperature due to the improved solubility. It was also found that acetamidines containing shorter hydrophobic tail tend to be more temperature-insensitive in the protonation process. However, as for the deprotonation process (N 2 bubbling), the as-formed acetamidines bicarbonates with short hydrophobic tails displayed evident temperature sensitivity, and thus higher temperature favored the regeneration of acetamidines. Additionally, the acetamidine bicarbonates with longer hydrophobic tails showed remarkable surface activity in the hexadecane/water emulsion than those with shorter hydrophobic tails. Furthermore, higher temperature and longer standing time accelerated the N 2 -triggered demulsification and the recovery of oil phase. The temperature sensitivity could allow these acetamidines to be deployed in CO 2 -triggered enhanced oil recovery (EOR).
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ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Wenqiong Li,Guanbo Wang,Rongbin Sun,Siyu Xu,Shanbin Luo,Yun He,Zeyi Lu,Bingtian Dong,Vellaisamy A.L. Roy,Xiaoguang Liang
Highly crystalline Cu–Sn alloy nanoparticles are prepared by CVD. • Tuned Cu:Sn ratio yields Cu 3 Sn and Sn/CuSn catalysts. • Cu 3 Sn shows high FE for HCOOH (75.5%) and CO (12.06%). • In situ Raman and DFT reveal CO 2 RR pathway and synergistic effects. The development of catalysts for the selective electrochemical CO 2 reduction reaction (CO 2 RR) has attracted increasing interest. In particular, Cu-based alloy catalysts, known for their superior stability and high catalytic activity, show great potential for CO 2 RR. Therefore, in this work, we prepared highly crystalline Cu–Sn alloys nanoparticles using a simple chemical vapor deposition (CVD) method. By controlling the Cu:Sn ratio, highly crystalline Cu 3 Sn and Sn-coated CuSn (Sn/CuSn) catalysts were obtained. Cu 3 Sn preferentially grows along the (210) facet, making the atomic distribution of Cu and Sn on this dominant surface play a crucial role in CO 2 RR performance. Owing to the synergistic effect between Cu and Sn, Cu 3 Sn exhibits high Faradaic efficiency (FE) for HCOOH (75.5%) and CO (12.06%) as compared to Sn/CuSn. Furthermore, the CO 2 RR evolution path and synergistic effects were revealed through in situ Raman spectroscopy and density functional theory (DFT) calculations, respectively. This work demonstrates the synthesis of highly crystalline Cu 3 Sn alloy nanoparticles and provides insights into the relationship between ordered Cu–Sn structures and CO 2 RR performance. Highly crystalline Cu 3 Sn nanoparticle catalyst was prepared using a combination of magnetron sputtering and chemical vapor deposition techniques. This catalyst features unique Cu and Sn active sites than enhance electrocatalytic performance through synergistic effects, enabling efficient CO 2 reduction to HCOOH and CO. Download: Download high-res image (211KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Jiangyong Yuan,Chunqiang Lu,Zhenhua Gu,Jun Cai,Han Zhao,Danyang Li,Lei Jiang,Haiwen Xu,Zhi qiang Li,Kongzhai Li
Carbon cycling, instead of conventional oxygen cycling in chemical looping, overcomes the limitations of oxygen storage capacity of oxygen carriers and enables the reaction to proceed under relatively mild conditions. In this study, we designed a high-performance carbon-storage catalyst (Ni-Co/Al 2 O 3 ) for chemical looping conversion of CH 4 and CO 2 to H 2 and CO. The physico-chemical characterizations suggested that the Co alloyed with Ni could result in larger active metal particles and simultaneously benefit the bending of carbon deposits toward the periphery of the active sites, avoiding the quick deactivation of catalysts due to the encapsulation of the active sites by carbon deposits and generating a higher carbon capacity (23.59 vs. 14.08 mol/kg). In addition, the alloying of Co with Ni could weaken the graphitization of carbon deposits, thus facilitating the carbon elimination and catalyst regeneration in the CO 2 conversion step, strongly improving the cycling stability during long-term testing.
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JACS Au
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2023
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IF 8
Jiajun Zhang,Kai Feng,Zhengwen Li,Bin Yang,Binhang Yan,Kai Hong Luo
Synthetic fuels produced from CO2 show promise in combating climate change. The reverse water gas shift (RWGS) reaction is the key to opening the CO2 molecule, and CO serves as a versatile intermediate for creating various hydrocarbons. Mo-based catalysts are of great interest for RWGS reactions featured for their stability and strong metal–oxygen interactions. Our study identified Mo defects as the intrinsic origin of the high activity of cluster Mo2C for CO2-selective hydrogenation. Specifically, we found that defected Mo2C clusters supported on nitrogen-doped graphene exhibited exceptional catalytic performance, attaining a reaction rate of 6.3 gCO/gcat/h at 400 °C with over 99% CO selectivity and good stability. Such a catalyst outperformed other Mo-based catalysts and noble metal-based catalysts in terms of facile dissociation of CO2, highly selective hydrogenation, and nonbarrier liberation of CO. Our study revealed that as a potential descriptor, the atomic magnetism linearly correlates to the liberation capacity of CO, and Mo defects facilitated product desorption by reducing the magnetization of the adsorption site. On the other hand, the defects were effective in neutralizing the negative charges of surface hydrogen, which is crucial for selective hydrogenation. Finally, we have successfully demonstrated that the combination of a carbon support and the carbonization process synergistically serves as a feasible strategy for creating rich Mo defects, and biochar can be a low-cost alternative option for large-scale applications.
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PubMed
高影响因子
LANGMUIR
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2023
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IF 3.9
Meisi Chen,Mengjia Li,Yinchun Liang,Weimin Meng,Zhibing Zhang,Youting Wu,Xinyao Li,Feng Zhang
Polyamines have emerged as a promising class of CO2 absorbents due to their remarkable sequestration capacity. However, their potential industrial application as aqueous absorbents is significantly hindered by a low regeneration efficiency and high energy consumption. To address these issues, this study investigates the use of triethylenetetramine (TETA) and ethylene glycol (EG) to develop a nonaqueous absorbent. The incorporation of EG enhances absorption performance and reduces the regeneration energy needed for TETA, whereas the high viscosity of the absorbent impedes absorption rate, amine efficiency, and regeneration efficiency. In order to enhance CO2 capture, micron-sized reaction units (SiO2@TETA-EG) were developed by encapsulating TETA solution with nanosilica. The SiO2@TETA-EG composite exhibits a large specific surface area (99 m2/g), with a porous shell structure and improved fluidity, which effectively counteracts the negative effects caused by high viscosity. Notably, SiO2@TETA-EG indicates a noticeably higher apparent rate constant of 4.29 min–1 at 323.2 K compared to the TETA-EG solution. Furthermore, SiO2@TETA-EG displays a 28.4% boost in regeneration efficiency while maintaining favorable stability in pore size and shape after regeneration.
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PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2023
·
IF 5.2
Bing Yao,Yuqi Wang,Zhou Fang,Yue Hu,Zhizhen Ye,Xinsheng Peng
Due to increased CO 2 emissions from the combustion of fossil fuels, considerable efforts have been made in CO 2 capture. The preparation of a membrane with higher mechanical qualities and large CO 2 adsorption capacity, however, remains the main obstacle. Here, using an in-situ anodic electrodeposition approach, we grow HKUST-1 MOFs into the graphene oxide (GO) two-dimensional (2D) nanochannels. A three-stage mechanism for the confined growth of MOFs during electrodeposition has been proposed. Through the inventive layer-by-layer confinement structural growth, MOFs@GO composite membranes with hierarchical pore structure were prepared. An extremely high CO 2 adsorption capacity of 194.1 cm 3 /g and CO 2 /N 2 adsorption ideal selectivity of 276.5 were achieved at 273 K and atmospheric pressure because of the synergistic effect of nanoconfined HKUST-1 and GO. The composite membrane prepared by electrodeposition method can expose more metal active sites in the presence of hierarchical porous structures, thus enhancing the CO 2 adsorption capacity. In addition, incorporating the HKUST-1 into GO nanochannels demonstrates 50.6% and 138.13% improvement in hardness and elastic modulus over pristine GO membrane, respectively. This provides a promising method for developing high-performance CO 2 capture membrane system under normal temperature and pressure conditions. It is also generally applicable for growing other MOFs@GO composite membranes, such as Cu-BDC@GO and Cu-BDC-NH 2 @GO membranes, respectively, and more suitable for large-scale industrial production.
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高影响因子
ENERGY
·
2023
·
IF 9
Hongming Fu,Yubin Shen,Zhaohao Li,Heng Zhang,Haiping Chen,Dan Gao
The application of membrane absorption for CO 2 capture has been limited by membrane wetting. In this paper, tubular Al 2 O 3 ceramic membranes (marked as M1 and M2) are hydrophobically modified by sol-gel and dip-coating method and then used for CO 2 capture. The surface morphology , surface composition, wettability and flux are characterized in detail. The mass transfer performance of M1 and M2 is studied at different gas and liquid Reynolds numbers . After modification, the surface contact angle can reach as high as 170.7°. The carbon capture performance of the modified M1 and M2 is significantly improved. Under laminar flow condition , CO 2 mass transfer coefficient increased from the initial 1.03 × 10 −4 m/s to 14.59 × 10 −4 m/s, and the CO 2 capture efficiency increased from the initial 28.55%–98.55%. The mass transfer resistance of ceramic membrane contactor is also analyzed. The resistance of liquid phase plays a leading role in the mass transfer performance in laminar flow state . For non-wetting membrane, membrane thickness has little effect on the mass transfer performance. In addition, it is shown that the superhydrophobic M1 and M2 exhibit excellent corrosion resistance . The research in this paper shows that superhydrophobic ceramic membrane is more suitable for CO 2 capture in industrial production.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Cederick Cyril Amoo,Joshua Iseoluwa Orege,Qingjie Ge,Jian Sun
The versatility of carbon has made it propitious for catalyst fabrication across various sectors of heterogeneous catalysis. Herein, a fundamental insight into the effects of carbon-supports in CO 2 hydrogenation is established by facilely preparing and investigating diversely configured carbon supported Fe catalysts. Although the active component remains Fe, unique synergies attained over the Fe-carbon interfaces created an ambience disparate among the catalysts for enhanced activity and selective distribution. Generally, the carbons facilitated C–C coupling but more C 5 + hydrocarbons are observed in the products when there is a stronger interaction between the carbon support and Fe phases. The selectivity for C 5 + hydrocarbons reached the highest of ∼ 40 % in total hydrocarbon products when Fe and Na were encapsulated in carbon. Carbide formation was eased as a result of enhanced CO 2 adsorption by the carbon supports whereas some surface functional groups attached to carbon surfaces improved C–C coupling to olefins and heavy hydrocarbons. The results presented maintains carbon as a promising catalytic material while the emphasis on structure, configuration, and surface properties reveal essentials in designing carbon-based catalysts in heterogeneous catalysis.
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