FUEL
·
2022
·
IF 8.035
Huangyu Yan,Guojie Zhang,Ying Xu,Qiqi Zhang,Jun Liu,Guoqiang Li,Yuqiong Zhao,Ying Wang,Yongfa Zhang
In recent years, amine functionalized materials have attracted great interest as prospective solid adsorbents for CO 2 capture. However, the amine functionalization of traditional supports (such as SBA-15, etc.) can lead to a decrease in the pore volume and specific surface area of the adsorbent, which significantly affects the CO 2 adsorption–desorption kinetics. To overcome this problem, the macro-/mesoporous multimodal pore silica was quickly synthesized using a ternary nonionic surfactant as a template through a partitioned collaborative self-assembly method, and impregnated with TEPA. The prepared support HMS-4 h has bimodal pores (pore size of 9.41 nm and 90 nm), which can not only improve the dispersibility of the loaded TEPA, but also effectively reduce the diffusion resistance of CO 2 . At the same time, the high surface area (838 m 2 /g) and large pore volume (2.34 cm 3 /g) of HMS-4 h can further improve the adhesion and quantity of amine-based active sites. The highest adsorption capacity reaches 6.04 mmol/g for HMS-4 h-75%TEPA at 90 ℃ and 1 bar. The adsorption capacity for HMS-4 h-75%TEPA was steady after 10 adsorption–desorption cycles. BET, XRD, FT-IR, SEM, TG-DTG were used to characterize the performance of the adsorbent. The CO 2 adsorption mechanism and the effects of organic amine loading, adsorption temperature and CO 2 concentration on CO 2 adsorption performance were systematically studied. The research shows that HMS-4 h-75%TEPA is an excellent adsorbent with high adsorption capacity in a wide temperature range, and low energy. This provides a reference for the design of high-performance solid amine CO 2 adsorbents in the future.
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高影响因子
GREEN CHEMISTRY
·
2022
·Vol. 24
·期 4
·1561-1569
·
IF 11.034
Peixuan Wu,Xinchao Wang,Ruhui Shi,Haiyang Cheng,Fengyu Zhao
The synthesis of self-healing and recyclable polymeric materials from renewable CO2 is of great importance in the fields of functional materials and sustainable chemistry. In this work, mechanically robust poly(urea-imine) (PUI) thermosets were prepared from CO2-sourced oligourea (OUa), terephthalaldehyde (TA) and tri(2-aminoethyl)amine (TAEA) through condensation between equimolar amino and aldehyde groups. The synthesized PUIs have satisfactory mechanical performance, seal-healing and recyclable properties as they contain cross-linked dynamic imine bonds and reversible hydrogen bonds. These properties can be adjusted by changing the ratio of TAEA to OUa, thus varying the chemical bonds and chain structure. The highest values for the mechanical properties tensile stress (10.2 MPa) and Young's modulus (79 MPa) were obtained in a PUI thermoset synthesized from a molar ratio of TAEA to OUa of 3 : 2 (OUa2-T3). In addition, this thermoset can be healed at 80 °C with a healing efficiency over 92% owing to the high reversibility of imine and hydrogen bonds and the flexibility of CO2-sourced OUa chains. Moreover, it can also be reprocessed and recycled by physical and/or chemical means without change in its chemical structure, glass transition temperature and original mechanical properties. Additionally, this PUI thermoset can be easily degraded into its original reagents OUa, TA and TAEA under acid conditions. Therefore, as novel sustainable materials, the PUI thermosets reported in this article have great potential to replace conventional non-degradable thermosets over a wide field.
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高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200188
·
IF 9.14
Chengjin Li,Xiaoxia Zhou,Qingming Zhang,Yi Xue,Zhaoyu Kuang,Han Zhao,Chung-Yuan Mou,Hangrong Chen
Graphical CO 2 to formic acid : A novel kind of Sn/TiO 2 /Si photocathode is developed for CO 2 reduction reaction (CO 2 RR), which shows excellent selectivity to HCOOH under applied potential. The improved light performance and heterojunction composite structure, together with the modulated electronic configuration, co-contribute to the high CO 2 RR performance. Using renewable energy to convert CO 2 into liquid products, as a sustainable way to produce fuels and chemicals, has attracted intense attention. Herein, a novel heterostructured photocathode composed of Si wafer, TiO 2 layer, and Sn metal particles has been successfully fabricated by combining of a facile hydrothermal and electrodeposition method. The obtained Sn/TiO 2 /Si photocathode shows enhanced light absorption performance by the surface plasmon resonance effect of Sn metal. Especially, the Sn/TiO 2 /Si photocathode together with rich oxygen vacancy defects jointly promote photoelectrochemical CO 2 reduction, harvesting a high faradaic efficiency of HCOOH and a desirable average current density (−4.72 mA cm −2 ) at −1.0 V vs. reversible hydrogen electrode. Significantly, the photocathode Sn/TiO 2 /Si also shows good stability due to the design of protecting layer TiO 2 . This study provides a facile strategy of constructing an efficient photocathode to improve the light absorption performance and the electron transfer efficiency, exhibiting great potential in the CO 2 reduction.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yafei Sang,Zhe Shu,You Wang,Lizhi Wang,Du Zhang,Qin Xiao,Fa Zhou,Jianhan Huang
A series of bifunctional ionic hyper-cross-linked polymers were synthesized by the Friedel-Crafts reaction and ionic post-functionalization. The as-prepared polymers had high Brunauer-Emmett-Teller surface areas ( S BET , 623–1345 m 2 /g), considerable bifunctional ionic groups, namely bromide anions, and carboxyl groups. The polymer namely DHI-CSU-3-Br had a good CO 2 capture capacity (134 mg/g, 273 K, and 1.0 bar), moderate isotopic adsorption heat (28–38 kJ/mol), and excellent CO 2 cycloaddition ability. The catalytic experiments showed that 99% of propylene oxide was successfully converted to cyclic carbonate (70 °C, 0.1 MPa CO 2 , and 4 h). The catalytic activity of the polymer was easy to be recovered and it was repeatedly reused 5 times without significant reduction. This synthetic strategy for the preparation of the bifunctional ionic hyper-cross-linked polymers provided an alternative approach for CO 2 capture and catalytic conversion.
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Zhiyan Si,Cederick Cyril Amoo,Yu Han,Jian Wei,Jiafeng Yu,Qingjie Ge,Jian Sun
Catalytic conversion of CO 2 to high-value products is a crucial method to achieve targets of carbon dioxide emissions peak and carbon neutralization. However, realizing a controllable product distribution in a single CO 2 hydrogenation process is of great challenge. Herein, we prepared the CuFe nanoalloy catalyst that directly transforms CO 2 to alkanes using physical sputtering method in mild condition. The characteristic results show that the proximity between Cu and Fe is the crucial factor to tunable products among the different catalysts. The formation of unique coordination of FeCu 4 nanoalloys from high-energy sputtering process provides close interaction between Cu and Fe, which is favorable to formation of low carbon paraffin, however, a distant proximity and weak interaction will increase the selectivity of olefins and alcohols. This work provides a general strategy for tuning target chemicals and enriches the viewpoints in CO 2 hydrogenation.
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高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Jianping Sheng,Ye He,Ming Huang,Chaowei Yuan,Shengyao Wang,Fan Dong
Lead (Pb) halide perovskite quantum dots (PQDs) are promising candidates for the photochemical reduction of CO2. However, the intrinsically weak adsorption and activation toward inert CO2 molecules have seriously hindered their practical application. This study reports alternative Cs2CuBr4 PQDs for gas–solid phase photocatalytic CO2 reduction under simulated solar irradiation. Cs2CuBr4 PQDs exhibited CO2 photoreduction performance with CH4 and CO yields of 74.81 and 148.98 μmol g–1, respectively. In situ diffuse reflectance infrared Fourier transform spectra and density functional theory calculations cooperatively revealed the synergistic strengthening of microelectronic polarization in Cs2CuBr4 PQDs induced by surface-frustrated Lewis pair-like properties and intrinsic Cu d-band properties facilitated robust CO2 adsorption and activation. This study demonstrated the potential of Cs2CuBr4 PQDs as a platform for highly efficient CO2 photoreduction and provided a distinct concept for CO2 adsorption and activation based on the catalytic mechanism of Cu-based PQDs.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Xiaoyan Pei,Zhiyong Li,Huiyong Wang,Qiuju Zhou,Zuodong Liu,Jianji Wang
Surfactant-free microemulsions (SFMEs) have shown great potential in many aspects such as chemical reactions and material preparation. Ionic liquid (IL)-based SFME is a promising member in this family. However, switchable phase separation of nonaqueous IL SFMEs has not been reported up to now although it is of great importance for the separation of products and recycling of the systems. Herein, a new kind of CO2-responsive SFMEs composed of quaternary ammonium IL, dimethyl sulfoxide, and ethyl acetate has been developed. It is worth noting that the microemulsion can be reversibly switched between emulsification and complete phase separation upon alternative CO2 and N2 bubbling at atmospheric pressure. The microstructures and phase behavior of the systems before and after CO2 bubbling have been systematically studied by phase diagrams, electrical conductivity, dynamic light scattering, optical microscopy, and atomic force microscopy, respectively. Mechanism studies verify that the reversible switching is attributed to the generation and restoration of more hydrophilic carbamate salts from the reaction of CO2 with IL anions, which results in poor solubility of ILs in the nonaqueous microemulsions and thus reversible breaking and rebuilding of the microemulsions. Based on this unique phase behavior, the CO2-switchable SFMEs are used as a microreactor for room temperature synthesis of Zn-based metal–organic frameworks, and effective reaction and microemulsion recycling have been achieved. This study may provide a new strategy for the integration of reaction, separation, and recycling procedures to obtain sustainable chemical processes.
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Catalysts
·
2023
·Vol. 13
·期 5
·807
·
IF 3.9
Zhiping Zhao,Zhixia Wang,Yanbing Tong,Jinru Sun,Ming Ke,Weiyu Song
The search for inexpensive, environmentally friendly, and highly effective catalysts to activate C-H bonds in propane dehydrogenation (PDH) reactions is still a major challenge. Co-based catalysts have gained significant attention in recent years due to their excellent ability to activate C-H bonds and their high selectivity towards olefins, despite being a non-noble and environmentally unfriendly metal. However, further improvements are necessary for practical utilization, particularly in terms of activity and anti-carbon deposition capacity. In this study, we synthesized Al2O3nanorods with abundant pentacoordinated Al3+(Al3+penta) sites. The supported Co on the Al2O3nanorod (Co/Al2O3-NR) exhibited higher selectivity (>96% propylene selectivity) and stability (deactivation rate 0.15 h−1) compared to Co supported on an Al2O3nanosheet with fewer pentacoordinated Al3+sites. Various characterizations confirmed that Co(II) mainly exists as CoAl2O4rather than Co3O4in the form of Co/Al2O3-NR, which inhibits the reduction of Co(II) to Co0and accordingly improves catalyst stability.Keywords:propane dehydrogenation;metal oxide;alumina;spinel
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhixiu Yang,Xiu Wen,Xiaoxuan Guo,Yong Chen,Ruiping Wei,Lijing Gao,Xiaomei Pan,Jin Zhang,Guomin Xiao
The electrochemical CO 2 reduction to specific multi-carbon product on copper-based catalysts is subjected to low activity and poor selectivity . Herein, catalyst structure, morphology, and chemical component are systematically studied for bolstering the activity and selectivity of as-prepared catalyzers in this study. Dendritic fibrous nano-silica spheres favor the loading of active species and the transport of reactant from the central radial channel. Cu/DFNS with high dispersion active sites are fabricated through urea-assisted precipitation way. The coexistence of Cu(I)/Cu(II) induces a close combination of Cu active sites and CO 2 on the Cu/DFNS interface, promoting the CO 2 activation and C C coupling. The Cu–O–Si interface (Cu phyllosilicate) can improve CO 2 and CO attachment. Cu/DFNS show the utmost Faradaic efficiency of C 2 H 4 with a value of 53.04% at −1.2 V vs. RHE. And more importantly, in-situ ATR-SEIRAS reveals that the C C coupling is boosted for effectively producing C 2 H 4 as a consequence of the existence of *CO L , *COOH, and *COH intermediates. The mechanism reaction path of Cu/DFNS is inferred to be *CO 2 → *COOH → *CO → *CO*COH → C 2 H 4 . Our findings will be helpful to gain insight into the links between morphology, texture, chemical component of catalyzers, and electrochemical reduction of CO 2 , providing valuable guidance in the design of more efficient catalysts.
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PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 39
·2302530
·
IF 13.3
Xiaotong Li,Minkai Qin,Xiuju Wu,Xiangzhou Lv,Jianghao Wang,Yong Wang,Hao Bin Wu
Electrochemical CO 2 reduction reaction (CO 2 RR) is a promising strategy for waste CO 2 utilization and intermittent electricity storage. Herein, it is reported that bimetallic Cu/Pd catalysts with enhanced *CO affinity show a promoted CO 2 RR performance for multi-carbon (C2+) production under industry-relevant high current density. Especially, bimetallic Cu/Pd-1% catalyst shows an outstanding CO 2 -to-C2+ conversion with 66.2% in Faradaic efficiency (FE) and 463.2 mA cm −2 in partial current density. An increment in the FE ratios of C2+ products to CO for Cu/Pd-1% catalyst further illuminates a preferable C2+ production. In situ Raman spectra reveal that the atop-bounded CO is dominated by low-frequency band CO on Cu/Pd-1% that leads to C2+ products on bimetallic catalysts, in contrast to the majority of high-frequency band CO on Cu that favors the formation of CO. Density function theory calculation confirms that bimetallic Cu/Pd catalyst enhances the *CO adsorption and reduces the Gibbs free energy of the C C coupling process, thereby favoring the formation of C2+ products.
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高影响因子
RSC Advances
·
2023
·Vol. 13
·期 25
·17362-17369
·
IF 3.9
Zhe Zhang,Fanhao Kong,Bizhen Yuan,Yinnian Liao,Xiue Ren,Yu Hou
Solar-driven CO2 reduction into fuels and sustainable energy has attracted increasing attention around the world. However, the photoreduction efficiency remains low due to the low efficiency of separation of electron–hole pairs and high thermal stability of CO2. In this work, we prepared a CdO decorated CdS nanorod for visible light driven CO2 reduction. The introduction of CdO facilitates the photoinduced charge carrier separation and transfer and acts as an active site for adsorption and activation of CO2 molecules. Compared with pristine CdS, CdO/CdS exhibits a nearly 5-fold higher CO generation rate (1.26 mmol g−1 h−1). In situ FT-IR experiments indicated that CO2 reduction on CdO/CdS may follow a COOH* pathway. This study reports the pivotal effect of CdO on photogenerated carrier transfer in photocatalysis and on CO2 adsorption, which provides a facile way to enhance photocatalytic efficiency.
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高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Chen Yiming,Hou Zhanggui,Wang Chuan,Ma Xin,Yang Hong,Wang Wen,Zhou Ling,Zhang Yi
As well known, the industrial methanation process needs highly active and stable catalysts obtained from cheap and abundant elements. In this work, we propose a high-loaded Ni/Al 2 O 3 catalyst promoted by manganese. Among them, the 20Ni2Mn/Al 2 O 3 catalyst exhibits the best CO 2 conversion (90.5%) and excellent methanation stability at 250 °C. In addition, the roles of the Mn promoter on CO 2 conversion and selectivity were investigated in detail. The features of natural and promoted catalysts are described through XRD, XRF, BET, TEM, H 2 -TPR, CO 2 -TPD, and operando DRIFTS techniques. Based on various characterization results, the addition of Mn will greatly reduce the Ni particle size and improve the Ni dispersion on the alumina support. Furthermore, compared to the unpromoted catalyst, Mn promoted catalysts show better reducibility and have more medium basic sites. And these medium basic sites are favorable to the adsorption and activation of CO 2 . In-situ DRIFTS experiments for CO 2 methanation reveal that manganese could promote the monodentate carbonate hydrogenated to formate rapidly, which could be faster converted towards CH 4 , contributing to significantly improved activity of the Mn promoted Ni/Al 2 O 3 catalyst. Graphical Abstract
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