JOURNAL OF POWER SOURCES
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2017
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IF 6.395
Jin Li,Qian Zhang,Peng Qiu,Lichao Jia,Bo Chi,Jian Pu,Jian Li
La 2 NiO 4+δ (LN)-coated PrBa 0.5 Sr 0.5 Co 1.5 Fe 0.5 O 5+δ (PBSCF) composite cathode, designated as PBSCF-LN, for the intermediate temperature solid oxide fuel cells (IT-SOFCs) is prepared by solution infiltration , and investigated comparatively with single phase PBSCF cathode in the half and full cells using Ag and/or Pt paste as the current collector. Compared with Pt, Ag current collector results in a decrease of cathode polarization resistance ( R P ) by an order of magnitude, which suggests that Ag is electrocatalytically active and not suitable for the use of studying the cathode performance of IT-SOFCs. The R P value of PBSCF-LN cathode is significantly lower than that of PBSCF cathode, no matter whether Pt or Ag current collector is used for the measurement. High power densities ranging from 0.24 to 0.94 W cm −2 at temperatures between 600 and 750 °C are achieved using a full cell with PBSCF-LN cathode. Upon exposure to a CO 2 -rich atmosphere, carbonate particles are formed on the surface of PBSCF cathode, causing irreversible degradation of electrochemical performance. In contrast, the surface of PBSCF-LN cathode remains clean, and its performance degradation due to CO 2 adsorption is recoverable.
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Micro & Nano Letters
·
2017
·Vol. 12
·期 9
·633-637
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IF 0.723
Jianwu Sun,Lingxiao Li,Jie Shen,Xiaoteng Zhou,Junpei Li,Chengyou Kan
A new kind of poly(methyl methacrylate–butadiene–styrene) (MBS) core/shell latex nanoparticles with amine groups in the shell was prepared via multistep seeded emulsion copolymerisation of styrene, methyl methacrylate and N,N-diethylaminoethyl methacrylate (DEAEMA) onto the poly(styrene–butadiene) seed latex in the presence of anionic emulsifier, and their CO 2 -triggered coagulating properties were investigated. Results showed that the emulsion polymerisation could be performed smoothly, and the coagulating time of the amine-containing MBS latexes depended on the DEAEMA content and solid content. The MBS solid powder could be easily obtained by drying and grinding without any extra treatment after the coagulation. A coagulating mechanism of the in-situ opposite charge interaction and the transformation from sodium laurate to lauric acid was proposed, which was demonstrated by transmission electron microscopy, dynamic light scattering, surface tension and Zeta potential measurements. This facile and smart method might open up industrial potential in cost-effective and environment-friendly latex coagulation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Jibo Liu,Huijie Shi,Qi Shen,Chenyan Guo,Guohua Zhao
Aiming at improving the efficiency of photoelectrocatalytic (PEC) CO 2 conversion to methanol, a heterogeneous photoelectrocatalyst was prepared by covalently binding a Ru(II) metal-organic complex (Ru-Py) containing exposed pyridyl on the periodic TiO 2 nanotube arrays (TNTAs). PEC characterization indicated that the Ru-Py/TNTAs photocathode exhibited excellent PEC CO 2 reduction activity in aqueous solution. The initial CO 2 reduction potential on Ru-Py/TNTAs photocathode reached −0.4 V (vs. NHE) under simulated solar irradiation. The cathodic photocurrent response of Ru-Py/TNTAs in CO 2 -satuarated aqueous solution was about 1.79 mAcm −2 , which was 2.4 times that of TNTAs . It may be caused by the enhanced light absorption in the visible region originated from Ru-Py. Meanwhile, Ru-Py played an important role in accelerating the separation of photoinduced electron-hole pairs evidenced by the photoluminescence spectra. PEC CO 2 reduction test showed that 84.8 μmol methanol was produced with 63.9% faraday efficiency, 62.6 turnover number (TON) and 45% selectivity at −0.9 V under 8 h irradiation. Furthermore, the non-covalent bonded system only produced 41.3 μmol methanol indicating that the carboxylic covalent linking displayed excellent electron transfer efficiency and methanolization performance. The mechanism investigation revealed that the exposed pyridyl provided the active sites in forming pyridiniumformate intermediates confirmed by the differential UV–vis absorption ( ΔA ) spectrum, which was of great significance in the efficient CO 2 methanolization. The probable reaction pathway for catalytic CO 2 reduction to methanol was also proposed combining the possible intermediates detected by gas chromatography mass spectrometry (GCMS).
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2016
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IF 2.196
Jia-nan Zheng,Ming-jun Yang,Yu Liu,Da-yong Wang,Yong-chen Song
Cyclopentane (CP) is considered to be a potential co-guest molecule in carbon dioxide (CO 2 ) hydrate-based desalination. The experimental thermodynamic data of CO 2 -CP hydrates were measured for a salt solution, where CP was chosen as a hydrate promoter. Seven experimental cases (62 cycles) were studied with different molar ratios of CP/water (0, 0.0025, 0.005, 0.0075, 0.01, 0.02, and 0.03). Hydrate phase equilibrium data were generated using an isochoric method, and the hydrate saturations were calculated based on gas uptake. The results indicated that the increase in CP concentration significantly decreased the CO 2 hydrate equilibrium pressure to a certain limit; the hydrate saturation also decreased during this process. Also, it was determined that CP encouraged the formation of s-II double CO 2 -CP hydrates, which are different from s-I simple CO 2 hydrate. The CO 2 -CP guest provides a strengthened stability and moderate hydrate phase equilibrium conditions for hydrate-based desalination. The recommended optimal molar ratio of CP is 0.01 when the increase in equilibrium was more than 10 K, and the decrease in hydrate saturation was less than 2%.
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APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Fengqin Yin,Linzhou Zhuang,Xianyong Luo,Shuixia Chen
The nitrogen-rich polymer network (MF/PAM) was synthesized through interpenetration between the molecular chains of melamine-formaldehyde resin(MF) and polyacrylamide (PAM), to which the polyethylene imine (PEI) was grafted to obtain solid amine adsorbent (MF/PAM-g-PEI). Compared with MF , the swelling capacity of MF/PAM was greatly enhanced, it could swell rapidly and directly in water. Although the interpenetration of PAM into MF may reduce the porosity of MF/PAM, the CO 2 capture capacity of the solid amine adsorbents (MF/PAM-g-PEI) could still reach 2.8 mmol/g at 273 K. The adsorbents also exhibited promising adsorption kinetics and regeneration performances. The kinetics observation showed that the Avrami model could better descript the CO 2 adsorption process compared with the pseudo-first-order model and pseudo-second-order model. Meanwhile, the Avrami kinetic orders (n a ) range from 1.21 to 1.56, displaying that the both physisorption and chemisorption exist in the adsorption process and the PEI have successfully grafted onto the polymer network, which also can be confirmed by the adsorption activation energy value. After 18 adsorption-desorption recycles, the MF/PAM-g-PEI could preserve its initial capacity without any decrease. Our work provides a new method to achieve promising solid amine adsorbents with higher adsorption capacity and better regeneration performance.
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Nanoscale
·
2017
·Vol. 9
·期 44
·17593-17600
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IF 7.367
Min Wang,Xiangqian Fan,Lingxia Zhang,Jianjun Liu,Beizhou Wang,Ruolin Cheng,Mengli Li,Jianjian Tian,Jianlin Shi
Porous activated carbons (PACs) are promising candidates to capture CO2 through physical adsorption because of their chemical stability, easy-synthesis, cost-effectiveness and good recyclability. However, their low CO2 adsorption capacity, especially low CO2/N2 selectivity, has limited their practical applications. In this work, an optimized PAC with a large specific surface area, a small micropore size, and a large micropore volume has been synthesized by one-step carbonization/activation of casein using K2CO3 as a mild activation agent. It showed a remarkably enhanced CO2 adsorption capacity as high as 5.78 mmol g−1 and an excellent CO2/N2 selectivity of 144 (25 °C, 1 bar). Based on DFT calculations and experimental results, the coexistence of adjacent pyridinic N and –OH/–NH2 species was proposed for the first time to make an important contribution to the ultra-high CO2 adsorption performance, especially CO2/N2 selectivity. This work provides effective guidance to design PAC adsorbents with high CO2 adsorption performance. The content of pyridine N combined with –OH/–NH2 was further elevated by additional nitrogen introduction, resulting in a further enhanced CO2 adsorption capacity up to 5.96 mmol g−1 (25 °C, 1 bar). All these results suggest that, in addition to the well-defined pore structure, pyridinic N with neighboring OH or NH2 species played an important role in enhancing the CO2 adsorption performance of PACs, thus providing effective guidance for the rational design of CO2 adsorbents.
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JOURNAL OF SUPERCRITICAL FLUIDS
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2016
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IF 2.579
Dongdong Hu,Yingna Zhang,Mei Su,Lei Bao,Ling Zhao,Tao Liu
The low molecular weight, topological structure and end group removal are expected to enhance the CO 2 -philicity of poly(vinyl acetate) (PVAc), which is of great interest for expanding CO 2 applications as a green solvent. This work aims at investigating the effect of molecular weight ( M n ) of PVAc with different molecular chain structure on the CO 2 -philicity through dissolution behavior measurement and molecular modeling. Well-defined 3-armed and 4-armed R-core PVAc was synthesized by RAFT polymerization, and then the corresponding xanthate groups were removed. The CO 2 -philicity of multi-armed PVAc was found to be inferior to that of linear one at low M n . With increasing the M n from 1000 to 7000 g/mol, the cloud point pressures ( P c ) of multi-armed PVAc first decreased, reached a minimum at a given M n , and then increased, which was different from the variation trend of the P c of linear PVAc versus M n . In addition, removal of the xanthate groups could effectively enhance the CO 2 -philicity of PVAc, especially at low M n . Moreover, the molecular dynamics (MD) simulations on the interactions in polymer/CO 2 systems indicated that the multi-armed structure had different effects on the compatibility with CO 2 at different M n . At low M n , the polymer⿿polymer interaction was the main driving force deciding the CO 2 -philicity due to the significant difference in different molecular chain structures. At high M n , multi-armed structure enhanced the CO 2 -philicity due to the synergistic effect of moderate polymer⿿polymer interaction and large polymer⿿CO 2 interaction. The appropriate molecular chain structure could be selected to enhance the CO 2 -philicity of PVAc at a certain M n .
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PLoS One
·
2016
·Vol. 11
·期 7
·e0159802
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IF 3.057
Zhujian Huang,Pingxiao Wu,Beini Gong,Yaping Dai,Pen-Chi Chiang,Xiaolin Lai,Guangwei Yu
To achieve a satisfactory removal efficiency of heavy metal ions from wastewater, silane-functionalized montmorillonite with abundant ligand-binding sites (-NH 2 ) was synthesized as an efficient adsorbent. Ca-montmorillonite (Ca-Mt) was functionalized with 3-aminopropyl triethoxysilane (APTES) to obtain the APTES-Mt products (APTES 1.0CEC -Mt, APTES 2.0CEC -Mt, APTES 3.0CEC -Mt, APTES 4.0CEC -Mt) with enhanced adsorption capacity for Co 2+ . The physico-chemical properties of the synthesized adsorbents were characterized by spectroscopic and microscopic methods, and the results demonstrated that APTES was successfully intercalated into the gallery of Ca-Mt or grafted onto the surface of Ca-Mt through Si-O bonds. The effect of solution pH, ionic strength, temperature, initial concentrations and contact time on adsorption of Co 2+ by APTES-Mt was evaluated. The results indicated that adsorption of Co 2+ onto Ca-Mt, APTES 1.0CEC -Mt and APTES 2.0CEC -Mt can be considered to be a pseudo-second-order process. In contrast, adsorption of Co 2+ onto APTES 3.0CEC -Mt and APTES 4.0CEC -Mt fitted well with the pseudo-first-order kinetics. The adsorption isotherms were described by the Langmuir model, and the maximum adsorption capacities of APTES 1.0CEC -Mt, APTES 2.0CEC -Mt, APTES 3.0CEC -Mt and APTES 4.0CEC -Mt were 25.1, 33.8, 61.6, and 61.9 mg·g -1 , respectively. In addition, reaction temperature had no impact on the adsorption capacity, while both the pH and ionic strength significantly affected the adsorption process. A synergistic effect of ion exchange and coordination interactions on adsorption was observed, thereby leading to a significant enhancement of Co 2+ adsorption by the composites. Thus, APTES-Mt could be a cost-effective and environmental-friendly adsorbent, with potential for treating Co 2+ -rich wastewater.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Han Feng,Luotian Lv,Yankai Huang,Tong Li,Yao Liu,Yongqing Wang
Syngas has important industrial applications, and converting CO 2 to CO is critical for syngas production. Metal-organic frameworks (MOFs) have demonstrated significant potential in photocatalytic syngas conversion, although the impact of catalytic reactions on tunable H 2 /CO ratios remains unclear. Herein, we present a novel bimetallic NiCo-MOF catalyst, Ni 0.4 Co 0.6 , exhibiting high catalytic activity in syngas conversion due to the CO product self-drive effect. Our investigation, integrating experimental data with density functional theory (DFT) analysis, uncovers a high photocurrent response and a low charge-transfer resistance. Furthermore, the introduction of cobalt into Ni-MOF caused an upshift of the d -band center, which facilitated the conversion efficiency of *COOH intermediates, which has been identified as the rate-determining step in CO 2 conversion, resulting in increased CO yield. Additionally, the concentration of undesorbed CO rises, while CO co-adsorption diminishes the catalyst’s binding energy for *H, thereby enhancing H 2 generation. These combined effects contribute to a self-driven enhancement in the catalytic production of syngas. By adjusting the Ni/Co ratio, a tunable H 2 /CO ratio (0.21–0.85) was achieved, with Ni 0.4 Co 0.6 exhibiting optimal catalytic performance, yielding 17.6 mmol·g −1 ·h −1 gas products. This study provides a novel insight into the correlation between reaction products and catalyst design, offering a perspective on perspective on modulating syngas composition.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·
IF 3.7
Yi Jing Jia,Jin Quan Tao,Hao Ran Liu,Wen Bin Huang,Rongpeng Yao,Miaomiao Niu,Rongrong Li,Qiang Wei,Ya Song Zhou
To enhance the CO 2 hydrogenation activity and low-carbon olefin selectivity of Fe-based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al 2 O 3 catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H 2 -TPR, XPS, CO 2 -TPD, NH 3 -TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO 2 hydrogenation activity and low-carbon olefin selectivity of Fe/Al 2 O 3 catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron-rich active metal centers in the catalyst, facilitating the adsorption and activation of CO 2 , while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low-carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C 2+ hydrocarbon products. Under the synergistic effect of K and Co, the CO 2 conversion activity of the Fe-based catalyst significantly increased, achieving a CO 2 conversion rate of 37%, while the selectivity towards C 2 -C 4= increased to 31.9%.
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iScience
·
2024
·
IF 4.6
Baiqin Zhou,Zhida Li,Xinyue He,Chunyue Zhang,Shanshan Pi,Min Yang,Wei Zhang,Guifeng Li,Ziqi Zhang,Lu Lu
Synergetic management of waste activated sludge, heavy metals (HMs) and CO 2 for their valorization and cyclic utilization is rarely reported. Herein, we employed sludge-derived extracellular polymeric substances (EPS) and HMs in wastewater to fabricate a gas diffusion electrode (GDE) for electrochemical CO 2 reduction. This approach atomically dispersed Ni at each nanofiber of the GDE. Abundant N element in the EPS proved to play a key role in the formation of N x -Ni (mixture of N 3 -Ni and N 4 -Ni) sites for highly efficient CO 2 to CO conversion. The atomical Ni 3+ shows high catalytic activity. Direct gaseous CO 2 reduction in a membrane electrode assembly generated a current density up to 50 mA·cm −2 with CO:H 2 ratio of ∼100 and ∼75% FE CO under 2.69 cell voltage. This strategy takes advantage of all waste streams generated on site and consolidates traditionally separated treatment processes to save costs, produces value-added products and generates carbon benefits during wastewater treatment.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2024
·
IF 2.2
Xuyao Tang,Yang Wang,Junwei Cui,Ke Zhang,Shengshan Bi
In this work, n -hexane, cyclohexane and 2-methylpentane were selected to represent linear-alkane, cycloalkane and branched-alkane, respectively. Based on the dynamic light method (DLS), the viscosity, interfacial tension and diffusion coefficient of n -hexane/CO 2 , cyclohexane/CO 2 and 2-methylpentane/CO 2 systems under saturation condition were measured in order to explore the change trend of thermophysical properties of the systems with the same carbon atom number but different molecular structures. The experiments were conducted at the temperatures of 303, 343 and 383 K and at pressures up to 5.64 MPa. The expanded uncertainties（ k = 2）of dynamic viscosity, interfacial tension and diffusion coefficient were 3 %, 3 % and 4.4 % respectively. The experimental results show that n -hexane and 2-methylpentane with similar molecular structure have more similar value of the properties. The effects of different alkane structures on system viscosity, interfacial tension, and diffusion coefficient were explained at the molecular level through radial distribution function, interface thickness, and CO 2 coordination number. At 303.15 K and 4 MPa, the peak radial distribution function of CO 2 /cyclohexane is 1.845, which is greater than that of CO 2 /n-hexane and CO 2 /2-methylpentane molecules. It has been proven that the arrangement of CO 2 /cyclohexane is more orderly, resulting in higher viscosity and lower diffusion coefficient of the system. The interface thickness of CO 2 /cyclohexane is 6.13 nm, which is smaller than CO 2 / n -hexane (7.53 nm) and CO 2 /2-methylpentane (6.3 nm). The smaller the interface thickness, the more compact the structure, the stronger the intermolecular forces, and the greater the interfacial tension. At 303.15 K and 2 MPa, the number of CO 2 coordination sites within 1 nm around liquid phase alkanes is 3.96, which is smaller than 4.78 for cyclohexane and 6.62 for 2-methylpentane. Prove that the coordination number is directly proportional to the diffusion coefficient and inversely proportional to viscosity and interfacial tension.
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