LANGMUIR
·
2014
·
IF 4.384
Pingwei Liu,Weiqiang Lu,Wen-Jun Wang,Bo-Geng Li,Shiping Zhu
Cross-linked polymer particles were prepared via surfactant-free emulsion copolymerization of 2-(diethylamino)ethyl methacrylate (DEAEMA) and sodium methacrylate (SMA) using N,N′-methylenebis(acrylamide) (MBA) as a cross-linker. Generated particles are zwitterionic, possessing unique isoelectric points in the pH range of 7.5–8.0, which is readily tunable through CO2/N2 bubbling. The particles were found to be highly responsive to CO2/N2 switching, dissolving in water with CO2 bubbling and precipitating with N2 bubbling at room temperature. Pickering emulsions of n-dodecane were prepared using these particles as the sole emulsifier. These emulsions can be rapidly demulsified with CO2 bubbling, resulting in complete oil/water phase separations. Nitrogen bubbling efficiently re-emulsifies the oil with the aid of homogenization. The rapid emulsification/demulsification using CO2/N2 bubbling at room temperature provides these cross-linked zwitterionic particles with distinct advantages as functional Pickering surfactants.
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Huiyuan Cheng,Xuemei Wu,Manman Feng,Xiangcun Li,Guangping Lei,Zihao Fan,Dongwei Pan,Fujun Cui,Gaohong He
Developing diatomic catalysts (DACs) for the CO2 reduction reaction (CO2RR) has emerged as a promising leading-edge research area owing to their maximum atomic utility and more sophisticated functionalities. However, the proper design of DACs at an atomic level and an understanding of the synergistic mechanism of binary sites remain challenging. Herein, an N-rich carbon matrix with precisely controlled Ni/Cu dual sites is synthesized through the assistance of metal–organic frameworks. The as-prepared catalyst presents high CO Faradaic efficiency of over 95% from −0.39 to −1.09 V vs reversible hydrogen electrode (RHE) with the maximum value of 99.2% at −0.79 V vs RHE and long-term durability of 60 h electrolysis. Density functional theory studies reveal that the electronic redistribution and band gap narrowing induced by the adjacent NiN4 and CuN4 moieties enhance the electron conductivity and strengthen the bonding interactions between *COOH intermediates and Ni centers, thus lowering the overall reaction barriers and promoting CO generation.
✓ 已验证
DOI
高影响因子
ACS Applied Bio Materials
·
2020
·
IF 0
Xinke Kong,Panpan Gai,Feng Li
Biohybrid photoelectrochemical systems could combine the light-harvesting ability of semiconductor photocatalysts and the CO2-processing capability of biocatalysts to realize CO2 reduction. How to develop the energy-utilized model can be of importance for the mechanism exploration of photosynthesis. Here, a biohybrid photoelectrochemical system based on HCOO––CO2 circulation was developed to realize the conversion both of solar-to-electric energy and chemical-to-electric energy. The device consists of a TiO2 nanoparticle photoanode and a laser-scribed graphene/formate dehydrogenase biocathode, which was utilized for the formic acid oxidation and the biocatalysis reduction of CO2 to HCOO–, respectively. The as-proposed biohybrid photoelectrochemical system exhibits good performance with an open-circuit potential of 0.93 V and a maximum power output density of 76 μW cm–2. This ingenious strategy not only exploits a robust carbon circulation system for the conversion of solar energy but also provides a way of constructing complex artificial photosynthesis systems.
✓ 已验证
DOI
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2024
·Vol. 40
·期 3
·484-489
·
IF 3.1
Xiao Qi,Liu Ting,Zhou Qianhe,Li Liangyu,Chang Chuntao,Gao Dawei,Li Danyang,You Feifei
Photocatalytic CO 2 reduction driven by solar light is a green approach that can decrease the greenhouse effect induced by high CO 2 concentration in the atmosphere and generate carbon-based chemicals/fuels as well. In this paper, non-metal co-catalysts ZnO/ZnS type-II hetero-junction nanoparticles with a rough surface were prepared through a hydrothermal process. When used as a photocatalyst for CO 2 reduction, the optimal one showed good cycle stability and a higher yield rate of 27.8 µmol·g −1 ·h −1 for CO 2 conversion into CO. The outstanding catalytic activity originated from i) the rich interfaces between ZnO and ZnS in the nanoscale could significantly reduce the delivery path of carriers and improve the utilization efficiency of photo-excited electron/hole pairs and ii) enriched surface oxygen defects could supply much more reaction active sites for CO 2 adsorption.
✓ 已验证
DOI
高影响因子
APPLIED ENERGY
·
2018
·
IF 7.9
Yao Shen,Chenkai Jiang,Shihan Zhang,Jun Chen,Lidong Wang,Jianmeng Chen
The main issue related to the deployment of the absorption based technology for CO 2 capture is the intensive energy penalty. Biphasic solvent is regarded as a promising candidate for CO 2 capture due to its potential in significant reduction of the energy consumption. However, currently, the development of biphasic solvents relies on the intensity of solvent screening work. To address this issue, this work investigated the relationships between the solvent properties and CO 2 capture performance such as absorption capacity, phase separation behavior, kinetics, and thermodynamics. Ten primary/secondary amines and eight tertiary amines with different alkalinity ( pKa ) and hydrophobicity (Log P) were used as the main components of the biphasic solvent . Experimental results revealed that the tertiary amine’s alkalinity determines the absorption capacity of the biphasic solvent. The maximum CO 2 absorption capacity was achieved by the tested biphasic solvent with a tertiary amine of a pKa around 9.8. Compared with the tertiary amine, the primary amine’s hydrophobicity was more sensible to the phase separation behavior of the solvent. The low Log P value of the primary amine and the high Log P value of the tertiary amine befitted the phase separation. Kinetic analysis indicate that the total mass transfer resistance of the rich solution decreased with the increase in the Log P value of the tertiary amine. Interestingly, the highest enhancement factor was achieved by the tertiary amine (2-(diethylamino)ethanol) with the pKa of 9.79. Further increase of the tertiary amine’s pKa decreased the enhancement factor of the biphasic solvent. This was attributed to the limitation of mass transfer of tertiary amine from the upper phase to lower phase. Furthermore, thermodynamic analysis showed that the sensible heat and the latent heat of the solvents decreased and increased, respectively, with the increase of log P value of the tertiary amines. The lowest reaction enthalpy and heat duty of the tested biphasic solvents were 45.8% and 52% lower than those of the benchmark monoethanolamine solution, respectively. Overall, compared with the primary amine, the selection of the tertiary amine is more important to achieve a great performance for CO 2 capture. Therefore, the tertiary amine with a moderate pKa and Log P is beneficial to achieve a high absorption capacity, fast absorption rate, and low heat duty of the biphasic solvent.
✓ 已验证
DOI
高影响因子
Nano Energy
·
2019
·
IF 15.548
Changfan Xu,Kaiwen Zhang,Da Zhang,Shilei Chang,Feng Liang,Pengfei Yan,Yaochun Yao,Tao Qu,Jing Zhan,Wenhui Ma,Bing Yang,Yongnian Dai,Xueliang Sun
A reversible long-life hybrid Na-CO 2 battery is proposed by using Na 3 Zr 2 Si 2 PO 12 solid electrolyte as a separator, N-doped single-wall carbon nanohorns (N-SWCNH) as a catalyst and the saturated NaCl solution as an aqueous catholyte. The Na 3 Zr 2 Si 2 PO 12 ceramic not only has high Na + ion conductivity, but also prevents potential contamination from H 2 O and CO 2 to sodium anode, and avoids the internal short-circuit touch of Na dendrite with cathode, improving the safety of the battery. Benefiting from N dopants , unique internal and interstitial nanoporous structures, N-SWCNH have large surface area for discharge products accumulation, offer substantial structural defect sites for CO 2 adsorption and electron transfer , contributing to high catalytic activity and reversibility . Most importantly, the hybrid Na-CO 2 battery with aqueous electrolyte facilitates the dissolution of the insulated discharge product, which overwhelmingly improves the discharge and charge reactions kinetics. Na-CO 2 batteries exhibit a low charging voltage of 2.62 V and a small voltage gap of 0.49 V at a current density of 0.1 mA cm −2 , a superior discharge capacity of 2293 mAh·g −1 at a current density of 0.2 mA cm −2 , a high round trip efficiency of ~68.7% after 300 cycles. In-situ Raman and ex-suit XRD analyses convincingly show that NaHCO 3 and carbon are the main discharge products.
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Shunan Yin,Jinxian Zhao,Shiping Wu,Xuhui Wang,Yanhong Quan,Jun Ren
Electrochemical reduction of CO 2 to valuable chemicals using electricity from renewable sources is a promising approach to realize the carbon cycle. Here, a novel bimetallic nitrogen-doped carbon catalyst (M-N-C, where M denotes the metal) CoCu–N–C electrocatalyst has been synthesized by pyrolyzing a copper-doped cobalt(II) acetate–phenanthroline complex formed from the metal acetates and 1,10-phenanthroline dissolved in ethanol. The optimal CoCu–N–C catalyst with molar ratio of Cu/(Co + Cu) = 0.15 displayed superior performance, enabling a faradaic efficiency of CO production of 76.5% at an overpotential of 0.57 V as well as an increased CO current density of 8.48 mA cm −2 at −0.98 V versus reversible hydrogen electrode (far superior than the Co–N–C of 4.20 mA cm −2 and Cu–N–C of 0.07 mA cm −2 ) and a decreased charge-transfer resistance compared with Co–N–C and Cu–N–C catalysts. The addition of Cu, which serves as a structure promoter to improve the dispersion of Co, thereby providing sufficient Co-N x active sites for the electrochemical CO 2 reduction reaction (CRR). Moreover, doping Cu changes the electronic environment around Co slightly and promotes the charge transfer capability so that reduces the energy barrier of potential-limiting energy, thereby improving the CRR performance of catalyst.
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2020
·
IF 3.557
Yangguan Chen,Guorong Lin,Shuixia Chen
Amine-skeleton solid-amine materials are promising adsorbents for CO2 capture from flue gas. Here, a novel solid-amine microsphere was synthesized by cross-linking the skeleton poly(ethylenimine) (PEI) with ethylene glycol diglycidyl ether in a facile one-pot W/O emulsion system. The material had a remarkable CO2 adsorption capacity of 7.28 mmol/g in the presence of moisture at 20 °C, 0.1 bar. The highest ratio of breakthrough capacity to saturation capacity was ca. 84%. According to kinetic simulation, the Avrami kinetic model could better describe the adsorption process of CO2 under different temperatures, in which the value of R2 was above 0.99 and n was between 1 and 2, indicating that both physical and chemical adsorption mechanisms were performed during adsorption. Moreover, the material had a high swelling speed. Equilibrium was established within 30 s, and the swelling ratio was 271% at equilibrium. The saturated adsorbent could be easily regenerated with a regeneration efficiency of 94.63% after six cycles. The PEI microsphere appears to be a promising candidate material for CO2 capture from flue gas.
✓ 已验证
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2021
·Vol. 2021
·期 35
·3601-3610
·
IF 2.524
Shaozhong Li,Qing Guo,Jin Li,Yongke Hu,Jiayu Lin
Graphical The mesostructured Cu/AlZnO-9 catalyst with 15 wt % Cu was prepared for the hydrogenation of CO 2 to methanol. The well mesostructure increased the exposed Cu surface area and CO 2 adsorption sites, which accelerated the CO 2 conversion, and the ZnO in catalyst increased the generation of methanol. In addition, the well mesostructure heightened the stability of supported Cu catalyst due to the high dispersion of Cu nanoparticles. In this work, the mesostructured Cu/AlZnO catalysts were prepared for the CO 2 hydrogenation to methanol. Experimental results showed that the weight ratio of Al 2 O 3 and ZnO affected the morphology of the mesoporous AlZnO supports and surface properties of the mesostructured Cu/AlZnO catalysts. The AlZnO-9 (the Al 2 O 3 mass within the AlZnO support was 90 wt%) with loose spongy porous structure and high surface area facilitated the Cu nanoparticle dispersion. Thus, the Cu/AlZnO-9 catalyst showed higher exposed Cu surface area ( S Cu ) and more exposed CO 2 adsorption sites, which accelerated the CO 2 conversion. Meanwhile, the ZnO added into catalysts increased the strength of surface basicity and the surface concentration of Zn species, which promoted the catalytic activity of CO 2 hydrogenation to methanol. In addition, the well mesostructure heightened the stability of supported Cu catalyst due to the high dispersion of Cu nanoparticles.
✓ 已验证
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 19
·10347-10354
·
IF 2.936
Shuangshuang Hou,Shaolei Wang,Xuejun Long,Bien Tan
In order to achieve efficient CO2 capture, four novel microporous organic polymers, based on distinct polycyclic aromatic hydrocarbons such as fluoranthene, binaphthalene, naphthalene and phenanthrene, were successfully prepared by the solvent knitting method. N2 sorption isotherms indicate that these polymers are predominately microporous with ultrahigh BET surface area i.e., 1788 m2 g−1 for fluoranthene-based Polymer 1, 1702 m2 g−1 for binaphthalene-based Polymer 2 and objective CO2 uptake capacity of 24.79 wt% and 20.19 wt% (273.15 K/1.00 bar) respectively. While compared with the former two polymers, though 1227 m2 g−1 and 978 m2 g−1 are moderate in surface area, however the naphthalene-based Polymer 3 and phenanthrene-based Polymer 4 still exhibit CO2 adsorption of up to 17.44 wt% and 18.15 wt% respectively under the similar conditions. Moreover, the H2 storage and CH4 adsorption in these polymers can be 2.20 wt% (77.3 K/1.13 bar) and 2.79 wt% (273.15 K/1.00 bar). More significantly, the electron-rich PAHs are proved to be new building blocks that provide a wealth of chances to produce hypercrosslinked polymers with efficient gas adsorption capacity, which are greatly influenced by the porous nature of polymers. Given the merits including mild reaction conditions, low cost, high surface area, impressive gas absorption performance, high thermal stability, these polymers are considered to be promising candidates for CO2 capture and energy storage under more practical conditions.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jingyun Qian,Wenna Zhang,Xue Yang,Kexin Yan,Meikun Shen,Hongyue Pan,Hongjun Zhu,Lei Wang
Constructing the metal cation-mediated low-cost inorganic sorbent with high separation efficiency in CO 2 , N 2 , and CH 4 remains a major challenge. Herein, we developed a series of alkali metal cations (Na + , K + , Rb + , Cs + )-exchanged ERI zeolites and adopted in the separation process of CO 2 among the gas mixture. Among the ion-exchanged zeolites, the zeolite K-ERI showed a high adsorption volume of 70.84 cm 3 g −1 and an IAST selectivity of CO 2 /CH 4 : 6254, CO 2 /N 2 : 2872 at 298 K, respectively, far outweighed the reported metal cation exchanged zeolites. Combining powder X-ray diffraction crystallography and density functional theory calculations, we unequivocally unveiled that the metal cations located at s 8 r effectively tailored zeolite aperture, and metal cation-gas molecules interactions synergically restrained the pass-through capacity of CO 2 in ion-exchanged ERI framework. Such a unique host–guest interaction governed by metal cations in aluminosilicate zeolite ERI affords a general strategy for gas separation.
✓ 已验证
DOI
高影响因子
PROGRESS IN ORGANIC COATINGS
·
2022
·
IF 6.206
Jiao Wei,Yuanchuan Ma,Yuquan Cai,Jieyuan Zheng,Hong Fan
In this work, a self-emulsifying CO 2 -based polyol (LAPEC) was prepared by the terpolymerization of propylene oxide , allyl glycidyl ether and CO 2 , followed by thiol-ene click reaction with mercaptopropionic acid. And the carboxyl group was successfully introduced into LAPEC verified in 1 H NMR. LAPEC was served as both soft segments and internal emulsifiers for WPU . Meanwhile, γ-aminopropylmethyldiethoxysilane (KH902) was also employed to improve the mechanical properties of WPU . Compared to dimethylol propionic acid (DMPA), WPU emulsion prepared by LAPEC had smaller particle size and higher emulsification efficiency. And the performance differences between LAPEC-based WPU films (LWPUs) and DMPA-based WPU films (DWPUs) with different hard segment contents were studied. The stronger hydrogen-bonding interactions improved the tensile strength , toughness and thermal stability. Compared with DWPU, the tensile strength and the elongation at break of LWPU respectively increased from 17.8 to 21.1 MPa and from 302.3 % to 356.5 %, when their hard segment content was both maintained around 37 wt%. Meanwhile, due to rougher surfaces and more hydrophobic silicon clusters, LWPU had stronger surface hydrophobicity . Therefore, LAPEC can provide a new way to synthesize WPU with high toughness and can be potentially used for flexible substrate coatings in the future.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）