INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Jian Chen,PeiPei Zhao,Dandan Li,Lina Liu,He Li
There is still a significant challenge to realize the connection of CO2 capture and utilization. Herein, we demonstrate an efficient and energy-saving system for tandem utilization of captured CO2 in order to produce cyclic carbonates with aqueous amine (BPEI10,000) as a CO2 adsorbent and a Cu(II) complex-intercalated porous organic framework as a heterogeneous catalyst. The porous organic polymer Bp-POF-Cu synthesized by the Schiff base reaction with a hierarchical microporous/mesoporous structure could efficiently catalyze cycloaddition of CO2 with propylene oxide to afford a high turnover frequency of 1360 h–1. With the in situ-released CO2 from BPEI10,000 solution as feedstock, up to 95% yield of cyclic carbonate was obtained over Bp-POF-Cu with epichlorohydrin as the substrate. The obtained results revealed that the CO2 desorption from amine solution and the catalytic reaction were successfully integrated, which demonstrated that the captured CO2 could be directly converted to cyclic carbonates in high yield through this heterogeneous catalytic system. Thus, we postulate that the tandem CO2 capture and cycloaddition reaction system presented here could offer an important method toward the implementation of the linking between CO2 capture and utilization.
研究领域:
化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Zhiping Zhang,Xuejiao Li,Huanyan Xu
Layered perovskite-related GdBaFe 2 O 5+ δ (GBF) and GdBaFeCoO 5+ δ (GBFC) oxides are systematically studied as advanced air electrodes for intermediate-temperature solid oxide fuel cells (IT-SOFCs). The characterizations of the samples are gauged with the assistance of a variety of techniques, involving X-ray diffractometer (XRD), O 2 -temperature programmed desorption (O 2 -TPD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and Fourier transform infrared spectrometry (FT-IR). Results of XRD demonstrate that GBFC has the exact same crystal structure as that of GBF, which displays slight lattice shrinkage. Substitution of Co for Fe increases the TEC from 9.87 × 10 −6 K −1 and 16.6 × 10 −6 K −1 at 150–700 °C. GBFC shows the highest conductivity of 500 S cm −1 at 520 °C, which complies with the requirement for the cathode of the fuel cell. The polarization resistance ( R p ) values of GBF and GBFC are 0.33 Ω cm 2 and 0.07 Ω cm 2 at 650 °C, respectively. Moreover, a single cell based on Sm 0.8 Ce 0.2 O 1.9 (SDC) electrolyte-supported is indicative of a peak power density of 0.28 W cm −2 for GBFC cathode at 700 °C. This single cell also exhibits a superior operational stability utilizing dry hydrogen fuel at 600 °C during the tested 220 h. Electrochemical impedance spectroscopy (EIS) and relaxation time distribution (DRT) results are suggestive of the slowly decreasing oxygen reduction kinetics of GBFC cathode with the introduction of CO 2 or gaseous Cr species, which may be connected with the formation of carbonate or Cr depositions. Compared to classic materials, GBFC cathode shows very good electrochemical stability and CO 2 /Cr tolerance.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 6
·3202-3210
·
IF 9.3
Wanbin Lin,Yihang Li,Manish Singh,Huibin Zhao,Rui Yang,Pei-Chen Su,Liangdong Fan
Reversible solid oxide cells (RSOCs) hold enormous potential for efficient direct CO2 reduction or CO oxidation in terms of exceptional faradic efficiency and high reaction kinetics. The identification of an active fuel electrode is highly desirable for enhancing the performance of RSOCs. This study explores the use of a alkaline metal dopant (Na) to modify the perovskite oxide of Na2x(La0.6−xSr0.4−x)FeO3−δ (2x = 0, 0.10, 0.20) materials with powerful CO2 chemical adsorption capacity, high oxygen ion conductivity, and low average valence of Fe sites for CO2/CO redox reactions. The experimental results indicate that the cells with the NaLSF0.10 fuel electrode achieve a current density of 1.707 A cm−2 at 1.5 V/800 °C and excellent stability over 120 hours at 750 °C for pure CO2 electrolysis, approximately 33.4% improvement over the pristine sample. When operated under a mixed CO–CO2 atmosphere under RSOC mode, the cell outputs the performance of 1.589 A cm−2 at 1.5 V and 329 mW cm−2 at 800 °C, and demonstrates relatively durable operation over 25 cycles. The addition of low valence sodium ions with high basicity and low electronegativity reduces the oxygen vacancy formation energy, increases the concentration of oxygen vacancies and modifies the electronic structure of LSF, thus enhancing CO2 adsorption, dissociation processes and charge transfer steps as corroborated by the detailed experimental analysis. Combined with the acceptable anti-carbon deposition capability, we prove here a feasible strategy and provide new insights into designing novel electrodes for SOEC/RSOCs to effectively convert CO2 with potential for renewable energy storage.
研究领域:
材料科学
·
电化学
·
能源存储
·
固体氧化物燃料电池
✓ 已验证
DOI
高影响因子
TETRAHEDRON
·
2019
·
IF 2.379
Jingyuan Li,Qingwen Song,Hengxuan Zhang,Ping Liu,Kan Zhang,Junwen Wang,Dengsong Zhang
Chemical fixation of carbon dioxide under mild reaction conditions e.g. atmospheric pressure and low temperature depends upon the ability of catalyst. Herein, a synergistic catalytic scheme of silver sulfadiazine/ n Bu 4 NBr was described for the three-component reaction of propargylic alcohols, CO 2 , and monohydric alcohols. This catalytic system was demonstrated effectively to provide β-oxopropyl carbonates in excellent yields (up to 99% yield with 5 mol% catalyst). The method tolerated a wide scope of propargylic alcohols and monohydric alcohols under atmospheric CO 2 pressure and solvent-free conditions. The excellent catalytic performance was attributed to the synergistic catalysis confirmed by the careful experiments.
研究领域:
催化
·
有机化学
·
绿色化学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 8
·2864-2872
·
IF 6.119
Xiaoli Li,Yuan Tang,Yue Jiang,Manman Mu,Xiaohong Yin
A series of composites composed of Bi4O5Br2 and Fe-MIL were successfully fabricated for mimicking sunlight-driven photocatalytic reduction of CO2. Herein, Bi4O5Br2, as a modulator of solid acids, could turn NH2-MIL-101(Fe) into NH2-MIL-88B(Fe) completely at 0.07 wt% catalytic loading, where further addition could construct the corresponding composites of Bi4O5Br2 and NH2-MIL-88B(Fe). The highest activity in the photocatalytic reduction of CO2 was achieved at 7.96 μmol g−1 h−1 of CH4 at 3.28 wt% of Bi4O5Br2. Besides, this catalyst possessed high photostability during the recycling experiments and the mechanism of this process was thoroughly explored. This study provides a novel strategy employing solid acid modulators for regulating the structure and morphology of MOFs showing high activity and stability in the photocatalytic reduction of CO2 to CH4.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Longkai Pan,Li Yao,Hui Mei,Hongxia Liu,Zhipeng Jin,Shixiang Zhou,Minggang Zhang,Gangqiang Zhu,Laifei Cheng,Litong Zhang
In this study, a novel 3D Bi 2 S 3 /P-ZnO S-scheme gyroid metamaterial was prepared by 3D printing and the hydrothermal method. The unique gyroid macrostructure and nanoarray microstructure offer a large volume of active sites for the photothermal catalytic reaction, thus improving the overall utilization rate of light. ZnO obtained by sintering the precursor produces oxygen vacancies, primarily due to P doping. This enables it to have a photothermal effect. After loading Bi 2 S 3 , the photothermal effect of P-ZnO and Bi 2 S 3 is coupled, further increasing the surface temperature of composite structure and speeding up the reaction rate. P-ZnO and Bi 2 S 3 formed a S-scheme heterojunction, promoting the separation and transfer of photogenerated carriers. Under simulated sunlight, the CO and CH 4 yield of Bi 2 S 3 /P-ZnO S-scheme gyroid metamaterials are 8.87 and 1.49 μmol h −1 . These are 3.45 times and 4.65 times of P-ZnO gyroid structure, respectively. Through SEM, TEM, XPS, ESR and in-situ FTIR characterizations, the transfer paths of photogenerated carriers between heterojunctions were revealed, and the reaction paths of photothermal catalytic CO 2 reduction were explored. The co-design of 3D structure and material allows for a novel concept for further improving photothermal catalytic performance.
研究领域:
材料科学
·
化学工程
·
环境科学
·
纳米技术
✓ 已验证
DOI
高影响因子
Journal of the American Chemical Society
·
2020
·
IF 14.612
Xianhua Zhang,Chunlei Pei,Xin Chang,Sai Chen,Rui Liu,Zhi-Jian Zhao,Rentao Mu,Jinlong Gong
Modulating lattice oxygen in metal oxides that conducts partial oxidation of methane in balancing C–H activation and syngas selectivity remains challenging. This paper describes the discovery of distorting FeO6 octahedra in La1–xCexFeO3 (x = 0, 0.25 0.5, 0.75, 1) orthorhombic perovskites for the promotion of lattice oxygen activation. By combined electrical conductivity relaxation measurements and density functional theory calculations studies, this paper describes the enhancement of FeO6 octahedral distortion in La1–xCexFeO3 promoting their bulk oxygen mobility and surface oxygen exchange capability. Consequently, La0.5Ce0.5FeO3 with the highest FeO6 distortion achieves exceptional syngas productivity of ∼3 and 8 times higher than LaFeO3 and CeFeO3, respectively, in CH4 partial oxidation step with simultaneous high CO2 conversion (92%) in the CO2-splitting step at 850 °C. The results exemplify the feasibility to tailor the active lattice oxygen of perovskite by modulating the distortion of BO6 in ABO3, which ultimately influences their reaction performance in chemical looping processes.
研究领域:
材料化学
·
催化化学
·
能源化学
·
无机固体化学
·
化学工程
✓ 已验证
DOI
高影响因子
ARABIAN JOURNAL FOR SCIENCE AND ENGINEERING
·
2023
·Vol. 48
·期 12
·16471-16482
·
IF 2.9
Zainuddin Muhd Izzudin Fikry,Ahmad Abdul Latif,Subramaniam Reasmyraj R.
Carbon dioxide (CO 2 ) separation with membrane technology has become the focus of researchers over the past decades due to its lower energy consumption and cheaper alternative. Mixed matrix membrane (MMM) of poly(4-methyl-1-pentene) (PMP) with nano fumed silica particles was studied to determine the feasibility of using MMM to separate CO 2 from nitrogen (N 2 ) gas. The critical concentration of PMP (7 wt%) was utilized to form the membrane in this study in order to ensure the polymer chain entanglement occurs to form a dense structure. Agglomeration of particle can be observed on the surface with scanning electron microscopy (SEM) imaging with 10 and 15 wt% of nano fumed silica loading in PMP matrix. This observation is further confirmed with energy-dispersive X-ray (EDX) mapping across the cross-sectional area which shows clustered nano fumed silica particle with loading of 10 and 15 wt%. With 7.5 wt% filler loading and at 1 bar, the MMM seems to give the best gas permeance performance with CO 2 permeance of 4.62 GPU (100.54 Barrer) and N 2 permeance of 0.20 GPU (4.31 Barrer) which makes the highest ideal selectivity to be about 23, which was the highest ideal selectivity achieved in this study. Meanwhile, when the pressure was increased from 1 to 7 bar, the CO 2 permeability increased almost linearly followed by a steady decline in CO 2 /N 2 ideal selectivity.
研究领域:
膜技术
·
气体分离
·
高分子科学
·
纳米复合材料
·
环境工程
✓ 已验证
DOI
高影响因子
Science China-Materials
·
2024
·Vol. 67
·期 2
·473-483
·
IF 6.8
Guan Chen,Liao Yulong,Xiang Quanjun
Simultaneous optimization of surface and interlayer characteristics of graphite-phase carbon nitride (g-C 3 N 4 ) is crucial for enhanced photogenerated-carrier separation efficiency. Integration of distinct strategies with specific merits for constructing efficacious charge carrier transport pathways from bulk to surface faces challenges. Herein, we proposed a novel carboxyl functional group and potassium (K) ions co-modified g-C 3 N 4 for steering dynamic charge transfer processes. Specifically, carboxyl functional groups were grafted to the surface to substantially improve charge carrier dynamics through the driving force induced by its electron-withdrawing effects. Concurrently, K ions were inserted into the interlayers of g-C 3 N 4 to facilitate interlayer carrier transport by bridging adjacent layers. Such a bi-functional photocatalyst achieves 8.68-fold increase in CO yield compared wtih the pristine g-C 3 N 4 without any cocatalyst or sacrificial agent. This work provides a profound discernment into the directional transport of charge carriers within the surface and interlayers, and presents a promising approach for rational design of photocatalysts with remarkably efficient solar energy conversion.
研究领域:
光催化
·
材料科学
·
环境科学
·
纳米技术
·
化学工程
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Weiping Liao,Haoyi Lin,Mengdie Yin,Jiaxing Zhang,Zhiguo Zhu,Hongying Lü
The confinement of metal-based matrix such as clusters, particles and even isolated single atoms in zeolite framework was intensively reported, while it was highly untoward to realize this goal for non-metallic ions due to the mutually-exclusive electrostatic interaction between the zeolite framework with negative charges and non-metallic anions. Herein, confinement of iodide ions in Mg-Beta zeolites (I@Mg-Beta) was successfully accomplished via the methodology of structural reconstruction, whose physicochemical property, channel connectivity as well as the location of Mg 2+ and I - ions were investigated systematically. It was found that Mg 2+ ions were located in the zeolitic framework and I - ions were mainly confined in Mg-Beta zeolite via the electrostatic interaction with tetraethylammonium cations. The establishment of structure–function relationship in CO 2 cycloaddition reaction with epoxides indicated the presence of synergistic effect between framework Mg 2+ ions and confined I - ions. The immobilisation of halide ions onto a zeolite support enabled it the recoverable ability from reaction systems, giving rise to relatively stable reusability. The catalytic transformation of CO 2 cycloaddition with epoxides in this work was devoted to ameliorate environmental stress from anthropogenic greenhouse gases of CO 2 by means of elaborately constructing metallosilicate zeolite confined non-metallic catalysts with dual functions.
研究领域:
催化
·
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Rong Rong,Yanwei Sun,Taotao Ji,Yi Liu
Zirconium-based MOF (Zr-MOF) membranes have attracted widespread attention due to their highly tailorable pore aperture and adsorption behavior achieved by functional group decoration and ligand/cluster-missing defect regulation as well as extraordinary chemical/thermal stability. Nevertheless, it has remained a great challenge to further improve the separation performance of Zr-MOF membranes due to very limited available zirconium sources and heating modes. In this study, we prepared polycrystalline UiO-66 membranes exhibiting unprecedented CO 2 /N 2 selectivity (31.3). The use of layered ZrS 2 , a representative of transition-metal dichalcogenides (TMDCs), as zirconium source during tertiary solvothermal growth was found to be indispensable for improving the separation performance of UiO-66 membranes. As far as we know, the CO 2 /N 2 selectivity reported in this study was the highest among all pristine polycrystalline MOF membranes measured under ambient conditions. More importantly, our study highlighted the importance of concurrent metal source and fabrication process innovation in performance enhancement of polycrystalline MOF membranes.
研究领域:
材料科学
·
化学工程
·
膜技术
✓ 已验证
DOI
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Wu Xinhao,Guo Yanan,Sun Zengsen,Xie Fenghua,Guan Daqin,Dai Jie,Yu Fengjiao,Hu Zhiwei,Huang Yu-Cheng,Pao Chih-Wen,Chen Jeng-Lung,Zhou Wei,Shao Zongping
Electrochemical CO 2 reduction (ECR) is highly attractive to curb global warming. The knowledge on the evolution of catalysts and identification of active sites during the reaction is important, but still limited. Here, we report an efficient catalyst (Ag-D) with suitable defect concentration operando formed during ECR within several minutes. Utilizing the powerful fast operando X-ray absorption spectroscopy, the evolving electronic and crystal structures are unraveled under ECR condition. The catalyst exhibits a ~100% faradaic efficiency and negligible performance degradation over a 120-hour test at a moderate overpotential of 0.7 V in an H-cell reactor and a current density of ~180 mA cm −2 at −1.0 V vs. reversible hydrogen electrode in a flow-cell reactor. Density functional theory calculations indicate that the adsorption of intermediate COOH could be enhanced and the free energy of the reaction pathways could be optimized by an appropriate defect concentration, rationalizing the experimental observation.
研究领域:
材料科学
·
电化学
·
光谱学
·
催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）