ACS Applied Materials & Interfaces
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2023
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IF 9.5
Danyang Li,Hongpeng Zhang,Songze Xie,Hao Zhang,Huan Wang,Xiaohong Ma,Dawei Gao,Jian Qi,Feifei You
It is a promising strategy to effectively promote “carbon neutrality” by reducing CO2 to small energy molecules through photocatalysis technology. However, due to low light utilization and recombination of photogenerated carriers, photocatalysts usually have low activity and low selectivity for products. Herein, a hollow spherical ZnS/ZnO heterojunction with a spatial confinement effect photocatalyst was synthesized toward CO2 photoreduction through preciously controlling the nano-/microstructure. The local lattice distortions were introduced into the surface of the hollow ZnS/ZnO microsphere, which activated lattice oxygen and provided additional active reaction sites. Furthermore, the heterojunction constructed between ZnS and ZnO interfaces facilitated the separation of photoinduced charge carriers. Combined with the natural advantage of enhanced light capture and absorption for a hollow confined structure, as a result, the systemic design in the electronic and confined structures for the photocatalyst has brought an excellent CO2 reduction performance with a CO yield rate as high as 35.85 μmol g–1h–1 and durability under a 300 W Xe lamp irradiation without any sacrificial agent and cocatalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yining Zhang,Mengyang Xu,Weiqiang Zhou,Xianghai Song,Xin Liu,Jisheng Zhang,Songtao Chen,Pengwei Huo
Step-scheme (S-scheme) heterojunctions can efficiently promote the separation of photogenerated carriers while maintaining the strong oxidation/reduction ability of photocatalysts; thus, research attention on S-scheme heterojunctions is increasing year by year. In this study, the S-scheme ZnO@ZnIn 2 S 4 (ZnO@ZIS) heterojunction was prepared successfully. Then, electron spin resonance (ESR) characterization was applied to prove the successful construction of the S-scheme heterojunction. Photoluminescence (PL), time-resolved photoluminescence (TRPL), and photoelectrochemical experiments have demonstrated efficient interfacial charge transport in ZnO@ZIS. Finally, the mechanism of CO 2 activation and electron transport was investigated by in situ Fourier transform infrared spectroscopy (FT-IR) and discrete Fourier transform (DFT) calculation analysis. The 40-ZnO@ZIS composite showed the best activity under light, and its CO and CH 4 yields reached 39.76 and 3.92 μmol∙g −1 ∙h −1 , respectively. This study provides a solution for optimizing the photocatalytic reduction activity of semiconductor photocatalysts by constructing S-scheme heterojunction materials to improve the CO 2 reduction capacity.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Binze Zhang,Zhen Zhang,Lijie Zhang,Kaibin Tang,Changrong Xia
Solid oxide electrolysis cells (SOECs) are regarded as a promising technology to realize carbon neutrality since they can electrochemically convert CO 2 to CO. This communication reports a feasible structure of a metal-supported solid oxide electrolysis cell (Ms-SOEC) for CO 2 electrolysis, where a porous 430 stainless steel substrate is coated with perovskite oxide La 0.6 Sr 0.4 Fe 0.9 Mo 0.1 O 3-δ (LSFM) introduced by the infiltration method . The LSFM catalyst exhibits a uniform distribution and loose accumulation in the porous metal substrate. This Ms-SOEC with a structure of LSFM-430|YSZ|LSCF-SDC shows a current density of 0.90 A cm −2 at 800 °C and 1.5 V with an LSFM loading of 6.0 wt%. Meanwhile, a 10-times thermal cycling operation demonstrates good reliability of the configuration. Overall, the metal-based cathode, where 430 stainless steel acts as the mechanical support and infiltrated LSFM perovskite acts as the electrocatalyst for CO 2 electrolysis, could be a viable configuration of Ms-SOECs.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 9
·2312691
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IF 19
Wenkai Xu,Gui-Rong Zhang,Jiansong Wang,Hui Yu,Weiwei Zhang,Liu-Liu Shen,Donghai Mei
Efficient electron transfer from photosensitizer to catalytic sites is crucial for effective artificial photosynthesis, yet it remains a significant challenge. Herein, it is reported that simple fluorination of the organic linkers in the MIL-101(Fe) photocatalyst results in a remarkable threefold increase in the photocatalytic CO 2 -to-CO conversion rate (688 µmol g −1 h −1 ) compared to the pristine counterpart (230 µmol g −1 h −1 ). It is unveiled that, instead of directly modifying the electron structure of MIL-101(Fe), the fluorinated linkers enhance the interaction between the discrete photocatalyst and photosensitizer ([Ru(bpy) 3 ] 2+ , bpy = 2,2'-bipyridine) via hydrogen bonding, thereby facilitating their intermolecular electron transfer. Most importantly, it is also demonstrated that this performance boosting strategy can be applied to other Fe-based metal–organic frameworks (MOFs) photocatalysts such as MIL-53(Fe) and MIL-88(Fe). The present work not only underscores the fluorination of organic linkers as a generic promising approach to enhance the photocatalytic performance of MOF-based catalysts, but also holds significant implications for photosynthesis and catalytic processes reliant on intermolecular electron transfer as an important step.
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CERAMICS INTERNATIONAL
·
2023
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IF 5.2
Zhiyuan Liu,Qixuan Xiang,Hao Zhang,Xianglong Zhang,Hunjun Tan,Yaping Zhao
MgCo 2 O 4 is a promising electrode material in electrochemical energy storage devices. In this work, the supercritical CO 2 -assisted solvothermal (SCAS) method was applied to synthesize MgCo 2 O 4 nanomaterials for the first time. The crystallite size of the MgCo 2 O 4 prepared by SCAS was significantly smaller than the one prepared by the ethanol solvothermal method, reaching 9.0 nm at a CO 2 pressure of 16 MPa. The as-prepared MgCo 2 O 4 nanospheres exhibited a special spherical structure with abundant irregular pores and a high specific surface area of 69.9 m 2 /g. X-ray photoelectron spectroscopy demonstrated that the Co 3+ /Co 2+ ratio of the MgCo 2 O 4 was increased by the SCAS method and the mechanism of synthesizing MgCo 2 O 4 nanospheres was explored. In addition, the MgCo 2 O 4 electrode material prepared by the SCAS method exhibited a high specific capacitance of 741 F/g at 0.1 A/g. The results confirm that the SCAS method can synthesize ultrafine MgCo 2 O 4 nanoparticles with special morphology and high specific surface area, which are expected to be applied in high-performance electrode materials.
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International Journal of Applied Ceramic Technology
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2023
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IF 2.1
Fangyi Huang,Xiaoli Tang,Qin Zhang,Xingyu Huo,Yuanxun Li,Xian Jian,Hua Su
In this study, the microwave dielectric properties of Co 2+ -substituted BaZnP 2 O 7 ceramics prepared through conventional solid-state synthesis were investigated. X-ray diffraction, Rietveld refinement, energy-dispersive spectroscopy, and Raman spectroscopy all indicated that BaZn 1− x Co x P 2 O 7 ceramics sintered at 875°C were composed of a single phase. The lattice strain and crystallite size were estimated using Williamson–Hall (W–H) method. Both the scanning electron microscopy images and density measurements showed that Co 2+ ions had an effect on the grain growth and densification of ceramics. The microwave dielectric properties were influenced by the intrinsic and extrinsic factors that varied with the increase of x value. An optimal performance ( ε r = 7.62, Q × f = 600 45 GHz, and τ f = −74 ppm/°C) was achieved at x = .01. The porosity and relative density played a significant role in the dielectric constant ε r : the denser the ceramic structure, the larger the dielectric constant. The Q × f and τ f values were negatively correlated with the full width at half maximum of the Raman vibrational peak at approximately 1049 cm −1 . Moreover, the Q × f value was improved compared to that of the undoped BaZnP 2 O 7 ceramics. Therefore, cobalt ion substitution is an effective strategy to enhance the performance of microwave dielectric ceramics.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Liu Yang,Jiawei Chen,Ning Ma,Zhenchang Fang,Xinling Li,Zhen Huang
A novel diamine-based biphasic absorbent, 3-(Dimethylamine)-1-propylamine (DMAPA)-Sulfolane-Water, was proposed for equimolar CO 2 absorption with high absorption–desorption efficiency. To optimize the CO 2 capture performance of the proposed DMAPA-Sulfolane-Water biphasic absorbents, the phase separation experiments and the absorption–desorption cyclic experiments were conducted. The results indicated that the DMAPA-Sulfolane-Water biphasic absorbent could realize a liquid–liquid phase separation performance after CO 2 absorption with sulfolane as the phase splitter and generate a CO 2 -rich upper-phase and a CO 2 -lean lower-phase. An equimolar absorption (1.023 mol CO 2 /mol DMAPA), a high initial absorption rate (0.106 mol/(L*min)), a low viscosity (10.96 mPa . s) and a high CO 2 loading (3.68 mol/L) of the CO 2 -rich upper-phase, a high desorption efficiency (92 %), and high cyclic stability were obtained due to the interaction of the intramolecular primary and tertiary amino groups in DMAPA. The minimum volume percentage of the rich phase was as low as 32 % of the total volume. In addition, temperature was confirmed to be an essential factor in the absorption and desorption process. The species in the two phases after CO 2 absorption were identified by 13 C NMR, not only further identifying the CO 2 -rich upper-phase but also revealing the mechanism of equimolar absorption by the DMAPA-Sulfolane-Water biphasic absorbents because of the high carbon peak of carbamic acid (DMAPACOOH) in the upper-phase. The quasi-salting out effect and the improved polarity of the solvents were proved to trigger the phase separation.
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DALTON TRANSACTIONS
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2023
·Vol. 52
·期 35
·12543-12551
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IF 4
Hu Li,Yuandong Yan,Shicheng Yan,Zhentao Yu,Zhigang Zou
Strategies to efficiently activate CO2 by strongly inhibiting the competitive hydrogen evolution reaction process are highly desired for practical applications of the electrochemical CO2 reduction technique. Here, we assembled a core–shell In@InOxHy architecture on carbon black by one-step reduction of NaBH4 as a CO2-to-formate catalyst with high selectivity. The stable CO2-to-formate reaction originates from the creation of steritic frustrated Lewis pairs (FLPs) on the InOxHy shell with In–OVs (OVs, oxygen vacancies) Lewis acid, and In–OH Lewis base. During CO2 reduction, the electrochemically stable FLPs are capable of first capturing and stabilizing protons to protonate FLPs to In–H Lewis acid and In–OH2 Lewis base due to its strong steric electrostatic field; then, CO2 is captured and activated by the protonated FLPs to selectively produce formate. Our results demonstrated that FLPs can be created on the surface of oxyphilic single-metal catalysts efficient in accelerating CO2 reduction with high selectivity.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Weixin Kong,Ziwei Chen,Fan Liu,Kexuan Yang,Yao Shen,Shihan Zhang,Wei Li,Sujing Li
Extensive energy consumption is a challenge for developing industrial carbon capture absorbents. A novel amino functionalized ionic liquid (AFIL) organic solution, tetraethylene pentamine 5-amino-4-imidazolecarboxamide/n-propanol/ethylene glycol ([TEPAH][AICA]/NPA/EG), is considered as a promising absorbent due to its high CO 2 absorption capacity and low energy consumption. However, its industry application potential still needs to be further evaluated for carbon capture process. In this work, thermodynamics, kinetics and corrosive behavior of [TEPAH][AICA]/NPA/EG solution were investigated. The regeneration energy consumption was 2.30 GJ⋅t −1 CO 2 , which was 39.5% lower than the benchmark monoethanolamine (MEA) solution. The mass transfer reaction kinetic model was established, showing that the reaction between CO 2 and [TEPAH][AICA]/NPA/EG solution followed fast pseudo-first-order. The enhancement factor and reaction rate constant increased with the increase of absorption temperature, while they showed a decreasing trend with the increase of absorption loading. The relationship between the second-order rate constant and temperature was expressed as k 2 = 7.2075 × 10 8 exp - 3093.5 T . The activation energy was 25.72 kJ·mol −1 . During absorption process, the dominant mass transfer resistance gradually changed from gas phase to liquid phase. In addition, the absorbent presented non-corrosive behavior after saturated absorption, which was superior than the MEA absorbent for storage and transportation in the carbon capture technology. To be concluded, the above results showed that the [TEPAH][AICA]/NPA/EG solution owned great potential for future industrial application.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Shumin Hong,Ting Li,Min Xiao,Teerawat Sema,Hongxia Gao,Zhiwu Liang
The concept of phase change absorbents has been widely studied as a novel and low-energy consumption option for CO 2 capture. This work screened diethylene glycol dimethyl ether (DGM) from 17 physical solvent species as a better phase change accelerator for absorbents of 2-(methylamino)ethanol (MAE)-physical solvent-H 2 O. Then, the optimized mass ratio of 30:49:21 for MAE-DGM-H 2 O solution was investigated with phase change behaviors, CO 2 absorption–desorption performance, cyclic capacity, and energy consumption. The experimental results showed that the cyclic CO 2 capacity reached 1.32 mol/L and the CO 2 -rich phase made up only 50.4 % of the total volume for the 30 wt%MAE-49 wt%DGM-21 wt%H 2 O, as well as its regenerative energy consumption was 40 % lower than that of 30 wt% monoethanolamine (MEA) solution. Also, the viscosity and surface tension gap of the CO 2 -rich phase and CO 2 -lean phase for the optimized absorbent were studied. It was observed that those gaps increase with the increasing mass ratio of DGM. In addition, the possible phase change mechanism was proposed by using the dipole moment values of components calculated by Gaussian (B3LYP/6-31G) coupled with 13 C NMR spectra.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Wen Hou,Jun Cheng,Leiqing Hu,Yulun Wu,Junhu Zhou
CO 2 capture and storage technologies are crucial for environmental conservation and sustainable progress. To overcome the challenging trade-off between permeability and selectivity in polymeric CO 2 separation membranes , we innovatively fabricated mixed matrix membranes (MMMs) by introducing three different NbOF 5 2− anion-pillared porous metal–organic frameworks (MOFs), namely NbOFFIVE-2-Cu-i, NbOFFIVE-2-Ni-i, and NbOFFIVE-bpy-Ni. The CO 2 capture performance of the three MOFs was investigated for the first time, and the ideal adsorption solution theory (IAST) method was used to predict the CO 2 separation selectivity. Density functional theory (DFT) calculations confirmed that the interaction energy between NbOFFIVE-2-Cu-i and CO 2 is the highest among the three MOFs. This is due to the optimal pore dimensions and strong C δ+ … F δ− electrostatic interaction between the C atoms in CO 2 molecules and the F atoms in NOFFIVE-2-Cu-i. The introduction of the three MOFs into the MMMs led to an increase in CO 2 solubility, resulting in enhanced CO 2 permeability and selectivity. The MMM loaded with 2 wt% of NbOFFIVE-2-Cu-i exhibited exceptional CO 2 permeability and CO 2 /N 2 ideal selectivity values of 578 Barrer and 70, respectively, representing enhancements of 39 % and 29 % compared to neat membrane, and exceeding the upper bound established in 2019.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Meixue Zhao,Jianping Guo,Qingping Xin,Yanli Zhang,Xu Li,Xiaoli Ding,Lei Zhang,Lizhi Zhao,Hui Ye,Hong Li,Guangyu Xuan,Yuzhong Zhang
Membrane separation is a novel technology that has been widely studied for efficient CO 2 capture. This study aims to synthesize novel porous amino-functionalized nanosheets using PEI (polyethyleneimine) (PEI-F-Ce) and PEI-F-Ce/polyethylene oxide (PEO) mixed matrix membranes (MMMs). PEI-F-Ce nanosheets were prepared via the electrostatic self-assembly method, allowing for the adjustment of both lateral and pore sizes of the nanosheets by varying the PEI concentration. The MMMs loaded with 2 % PEI-F-Ce-2.5 nanosheets exhibit excellent CO 2 permeability (641 Barrer) and outstanding CO 2 /N 2 selectivity (70.1). These values surpassed those of pure PEO membranes by 62 % and 53 %, respectively, exceeding the 2019 upper bound. PEI-F-Ce-2.5 nanosheets with a stable pore channel 3.406 nm improved CO 2 transport and showed a large CO 2 adsorption capacity of 1.32 mmol g −1 , leading to enhanced the CO 2 /N 2 reaction selectivity. Moreover, the reversible reaction of CO 2 with –NH 2 enhanced the CO 2 /N 2 selectivity by 5.1 times at −20 °C, thereby highlighting its potential for cryogenic gas separation applications.
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