ACS Applied Materials & Interfaces
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2021
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IF 9.229
Meidan Que,Yang Zhao,Yawei Yang,Longkai Pan,Wanying Lei,Weihua Cai,Hudie Yuan,Jin Chen,Gangqiang Zhu
Metal halide perovskite with a suitable energy band structure and excellent visible-light response is a prospective photocatalyst for CO2 reduction. However, the reported inorganic halide perovskites have undesirable catalytic performances due to phase-sensitive and severe charge carrier recombination. Herein, we anchor the FAPbBr3 quantum dots (QDs) on Ti3C2 nanosheets to form a FAPbBr3/Ti3C2 composite within a Schottky heterojunction for photocatalytic CO2 reduction. Upon visible-light illumination, the FAPbBr3/Ti3C2 composite photocatalyst exhibits an appealing photocatalytic performance in the presence of deionized water. The Ti3C2 nanosheet acts as an electron acceptor to promote the rapid separation of excitons and supply specific catalytic sites. An optimal electron consumption rate of 717.18 μmol/g·h is obtained by the FAPbBr3/0.2-Ti3C2 composite, which has a 2.08-fold improvement over the pristine FAPbBr3 QDs (343.90 μmol/g·h). Meanwhile, the FAPbBr3/Ti3C2 photocatalyst also displays a superior stability during photocatalytic reaction. This work expands a new insight and platform for designing superb perovskite/MXene-based photocatalysts for CO2 reduction.
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Sustainable Energy & Fuels
·
2021
·Vol. 5
·期 11
·2871-2876
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IF 6.367
Ziling Liu,Yaqi Huang,Shuqing Chang,Xiaoli Zhu,Yanghe Fu,Rui Ma,Xinqing Lu,Fumin Zhang,Weidong Zhu,Maohong Fan
The visible-light driven photocatalytic conversion of CO2 into valuable hydrocarbons is a highly attractive approach for sustainable carbon cycle to solve the worldwide environmental and energy problems. Herein, highly dispersed Ru nanoparticles (NPs) are confined in a photosensitizing bipyridine-linked covalent organic framework (TpBpy) to facilely construct Ru@TpBpy composites. The resulting Ru@TpBpy catalysts exhibit significantly enhanced activities for CO2 reduction under visible-light irradiation, giving the maximum HCOOH production rate of 172 μmol gcat−1 h−1 over 0.7 wt% Ru@TpBpy. The interactions between Ru NPs and TpBpy can not only enhance the visible-light harvesting, but also restrain the recombination of photo-generated charges efficiently and facilitate the electron transfer through Ru NPs, thereby improving the photocatalytic performance for CO2 reduction. The current work provides a promising pathway to construct efficient photocatalysts with highly dispersed metallic NPs confined into photosensitizing COFs via utilizing the coordination microenvironments and also expands the application of COF-based materials.
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Journal of Coatings Technology and Research
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2021
·Vol. 18
·期 4
·989-998
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IF 2.382
Xu Liangfeng,Wang Zhaofei,Yang Gongwen,Zhang Guobing,Wei Haibing,Fang Huagao,Ding Yunsheng
Traditional waterborne polyurethane (WPU) has poor water resistance because of the incorporation of permanent hydrophilic groups, such as carboxyl group or ammonium salt, into polymer chains. Therefore, developing WPU with excellent water resistance and mechanical properties is highly desirable for industrial applications. In this study, CO 2 -triggered hydrophobic/hydrophilic switchable waterborne polyurethane–acrylate (WPUA) containing methyl methacrylate (MMA) units were designed and synthesized. The molecular structure, hydrophobic/hydrophilic switchable behavior, water resistance, and mechanical properties were systematically investigated and characterized. The WPUA with 10 wt% MMA exhibited a low water uptake (2.15 wt%) and linear swelling ratio (0.17 L%), as well as a high tensile strength (16.7 MPa) and modulus (85.9 MPa), which were much higher than those of the pristine WPU. This study indicated that the CO 2 -triggered WPUA dispersed stably as latex particles in water and possessed excellent water resistance and mechanical properties after the film formation.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Changming Zhang,Yaqi Wang,Xiaochao Zhang,Rongxian Wang,Lifang Kou,Jiancheng Wang,Rui Li,Caimei Fan
The increase of CO 2 adsorption and separation efficiency of photo-induced carriers are two crucial factors for achieving effective CO 2 reduction into solar fuels. Here, novel millimeter-level nitrogen modified resin-based activated carbon spheres (N-ACSs), as desired support to immobilize and tailor Bi 4 Ti 3 O 12 catalyst (Bi 4 Ti 3 O 12 /N-ACSs) for improving CO 2 photoreduction activities, have been constructed via simple suspension polymerization and impregnation method. The involved TG, FTIR, XRD, XPS, EA, SEM, EDS, N 2 adsorption/desorption, CO 2 adsorption, UV–vis DRS, MS, PC, EIS, PL spectra and in-situ FTIR were characterized. Bi 4 Ti 3 O 12 /N-ACSs displayed the highest photocatalytic CO 2 reduction activity to CO of 142.76 μmol/g under 8 h simulated sunlight irradiation in pure H 2 O phase, approximately 1.45 times and 1.24 times higher than that of pristine Bi 4 Ti 3 O 12 and Bi 4 Ti 3 O 12 /ACSs, respectively. The introduction of N-ACSs played four roles: (i) the increase of CO 2 adsorption, (ii) the red-shift of optical absorption range, (iii) the consummate separation and transfer of photo-induced carriers, (iv) more CO 2 active sites. Finally, the possible mechanism photocatalytic CO 2 reduction for Bi 4 Ti 3 O 12 /N-ACSs was proposed. Our findings should provide noteworthy promising strategy to immobilize powder photocatalyst on the surface of millimeter-level carbon spheres for achieving the high-efficient CO 2 adsorption and photoreduction to CO.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Lv Houfu,Lin Le,Zhang Xiaomin,Li Rongtan,Song Yuefeng,Matsumoto Hiroaki,Ta Na,Zeng Chaobin,Fu Qiang,Wang Guoxiong,Bao Xinhe
Metal nanoparticles anchored on perovskite through in situ exsolution under reducing atmosphere provide catalytically active metal/oxide interfaces for CO 2 electrolysis in solid oxide electrolysis cell. However, there are critical challenges to obtain abundant metal/oxide interfaces due to the sluggish diffusion process of dopant cations inside the bulk perovskite. Herein, we propose a strategy to promote exsolution of RuFe alloy nanoparticles on Sr 2 Fe 1.4 Ru 0.1 Mo 0.5 O 6− δ perovskite by enriching the active Ru underneath the perovskite surface via repeated redox manipulations. In situ scanning transmission electron microscopy demonstrates the dynamic structure evolution of Sr 2 Fe 1.4 Ru 0.1 Mo 0.5 O 6− δ perovskite under reducing and oxidizing atmosphere, as well as the facilitated CO 2 adsorption at RuFe@Sr 2 Fe 1.4 Ru 0.1 Mo 0.5 O 6− δ interfaces. Solid oxide electrolysis cell with RuFe@Sr 2 Fe 1.4 Ru 0.1 Mo 0.5 O 6− δ interfaces shows over 74.6% enhancement in current density of CO 2 electrolysis compared to that with Sr 2 Fe 1.4 Ru 0.1 Mo 0.5 O 6− δ counterpart as well as impressive stability for 1000 h at 1.2 V and 800 °C.
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Journal of CO2 Utilization
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2021
·
IF 7.132
Qin Ying,Han Chen,Peijing Shao,Xiaowei Zhou,Xiaojia He,Jiexu Ye,Shihan Zhang,Jianmeng Chen,Lidong Wang
Tertiary amine-based absorption process possesses high absorption capacity and low heat duty for CO 2 capture. However, its slow CO 2 absorption rate retards its industrial application. This work developed a core-shell magnetic ZIF-8@Fe 3 O 4 -carbonic anhydrase composite to promote CO 2 absorption into tertiary amine, e.g., diethanolamine (MDEA) due to its easy recovery from the solution. The catalytic performance of CA@ZIF-8@Fe 3 O 4 that had three particle sizes were investigated. Experimental results revealed that the obtained CA@ZIF-8@Fe 3 O 4 can achieve the relative activity as high as 95.2 % compared with the free counterparts. Large particle size of ZIF-8@Fe 3 O 4 was beneficial to activity but adverse to loading. Magnetic analysis shows that the developed CA@ZIF-8@Fe 3 O 4 possessed remarkable magnetic response which made recycling more convenient.
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Journal of Energy Chemistry
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2021
·
IF 9.676
Qiaojuan Wang,Yating Gao,Chantsalmaa Tumurbaatar,Tungalagtamir Bold,Fei Wei,Yihu Dai,Yanhui Yang
Carbonate-modified metal-support interfaces allow Ru/MnCO 3 catalyst to exhibit over 99% selectivity, great specific activity and long-term anti-CO poisoning stability in atmospheric CO 2 methanation. As a contrast, Ru/MnO catalyst with metal-oxide interfaces prefers reverse water–gas shift rather than methanation route, along with a remarkably lower activity and a less than 15% CH 4 selectivity. The carbonate-modified interfaces are found to stabilize the Ru species and activate CO 2 and H 2 molecules. Ru-CO* species are identified as the reaction intermediates steadily formed from CO 2 dissociation, which show moderate adsorption strength and high reactivity in further hydrogenation to CH 4 . Furthermore, carbonates of Ru/MnCO 3 are found to be consumed by hydrogenation to form CH 4 and replenished by exchange with CO 2 , which are in a dynamic equilibrium during the reaction. Modification with surface carbonates is proved as an efficient strategy to endow metal-support interfaces of Ru-based catalysts with unique catalytic functions for selective CO 2 hydrogenation.
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Journal of Natural Gas Science and Engineering
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2021
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IF 4.965
Xiangyu Cai,Ye Yuan,Menglong Sheng,Jixiao Wang,Zhi Wang
The polyvinylamine (PVAm) was respectively modified by the MOFs (IRMOF-3 and ZIF-8) with amine groups that were characterized by TEM, SEM and XRD . The PVAm-MOFs/polysulfone (mPSf) mixed matrix membranes (MMMs) were fabricated by coating different PVAm-MOFs mixtures on mPSf ultrafiltration membranes. The performance of the PVAm-MOFs/mPSf and PVAm/mPSf membranes for CO 2 /CH 4 separation was investigated. Compared with the PVAm/mPSf virgin membrane, PVAm-MOFs/mPSf MMMs display higher CO 2 separation performance due to the decreased membrane effective thickness and incorporation of amine-rich nanochannels. Furthermore, compared with PVAm-ZIF-8/mPSf MMM, the PVAm-IRMOF-3/mPSf MMM possesses higher CO 2 /CH 4 separation performance. Then the CO 2 /CH 4 separation performance of the PVAm-IRMOF-3/mPSf MMMs with different IRMOF-3 loadings was studied. Compared with other reported membranes, the PVAm-IRMOF-3/mPSf MMM loaded 25 wt% IRMOF-3 shows higher CO 2 /CH 4 separation performance at both low and high feed pressure.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Wanbo Zhang,Ping Guo,Xingbo Ge,Jianfen Du,Zhouhua Wang
In CO 2 enhanced oil recovery process, the interactions between CO 2 and oil components are complex since crude oil is a mixture of n-alkanes, cycloalkanes , aromatics, resin, asphaltene and other compounds. To investigate the effects of temperature, pressure and molecular structure on CO 2 solubility in cycloalkanes and the resulting cycloalkane volume expansion, the solubility of near critical and supercritical CO 2 in cyclopentane (CP), cyclohexane (CH), methylcyclohexane (MCH), methylcyclopentane (MCP) and ethylcyclohexane (ECH) and the volume expansion factor of cycloalkanes at diverse temperature and pressure were measured. It was observed that increasing temperature decreases CO 2 solubility, while CO 2 solubility increases with pressure increasing. Compared with CP and CH, it's harder for CO 2 to dissolve in their methyl or ethyl substituents. For homologues, CO 2 solubility decreases with carbon number increasing. The volume expansion factor and solubility have a same variation tendency with temperature, pressure and molecular structure. The experimental results of solubility were correlated with Fornari's model and PR equation of state with the maximum average absolute relative deviation (AARD) of 2.8% and 6.8%, respectively. The excess molar volume of CO 2 + cycloalkane mixtures was calculated to be negative and increases with pressure.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Yang Li,Zhi Liu,Zhao Li,Qiu Wang
Constructing noble metal-doped g-C 3 N 4 /carbon composites is a feasible route to overcome the intrinsic drawbacks of pristine g-C 3 N 4 for enhanced activity of CO 2 photoreduction. Herein, a novel Ag-doped g-C 3 N 4 /biomass-derived carbon composite with hollow bird's nest-like (Ag-g-C 3 N 4 /BN-C) is designed and prepared via a simple yet effective one-step pyrolysis method. In the Ag-g-C 3 N 4 /BN-C, the highly-dispersed Ag nanoparticles (20–30 nm) with the surface plasmon resonance (SPR) effect act as a significant cocatalyst not only to efficiently trap the photogenerated electrons from g-C 3 N 4 to boost the separation of photogenerated electron-hole pairs but also to produce additional active “hot electrons”, while the conductive quasi-spherical hollow structure of BN-C doubles the specific surface area with multiple reflections of light, providing abundant active sites and more utilization efficiency of light energy. As a result, the Ag-g-C 3 N 4 /BN-C exhibits a remarkably enhanced CO evolution rate of 33.3 μmol·g −1 ·h −1 without addition of any sacrificial reagents and photosensitizers, superior to those of both the pristine g-C 3 N 4 and many reported g-C 3 N 4 -based counterparts. The findings of this work demonstrate a good indication for integrating g-C 3 N 4 with SPR-dependence noble metal and renewable biomass-derived carbon for enhanced CO 2 photoreduction, which may be extended to modify other semiconductor materials for more photocatalytic applications with enhanced activity.
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CHEMISTRY-A EUROPEAN JOURNAL
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2021
·Vol. 27
·期 62
·15536-15544
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IF 5.236
Li-Qi Qiu,Kai-Hong Chen,Zhi-Wen Yang,Fang-Yu Ren,Liang-Nian He
Graphical CO 2 photoreduction : A series of new mononuclear rhenium(I) complexes with imidazole-pyridine framework based on the long-lived excited triplet state exhibit satisfactory stability and catalytic efficiency in photoreduction of CO 2 to CO. This work emphasizes the practice and importance of tailored photocatalyst design on molecular level, representing appealing and potentially applications for phosphorescent catalysts in CO 2 reduction to solar fuels. The photocatalytic reduction of CO 2 into fuels offers the prospect for creating a new CO 2 economy. Harnessing visible light-driven CO 2 -to-CO reduction mediated by the long-lived triplet excited state of rhenium(I) tricarbonyl complexes is a challenging approach. We here develop a series of new mononuclear rhenium(I) tricarbonyl complexes ( Re-1 − Re-4 ) based on the imidazole-pyridine skeleton for photo-driven CO 2 reduction. These catalysts are featured by combining pyridyl-imidazole with the aromatic ring and different pendant organic groups onto the N1 position of 1,3-imidazole unit, which display phosphorescence under Ar-saturated solution even at ambient conditions. By contrast, {Re[9-(pyren-1-yl)-10-(pyridin-2-yl)-9H-pyreno[4,5-d]imidazole)](CO) 3 Cl} ( Re-4 ) by introducing pyrene ring at the N1 position of pyrene-fused imidazole unit exhibits superior catalytic performance with a higher turnover number for CO (TON CO =124) and >99.9 % selectivity, primarily ascribed to the strong visible light-harvesting ability, long-lived triplet lifetimes (164.2 μs) and large reductive quenching constant. Moreover, the rhenium(I) tricarbonyl complexes derived from π-extended pyrene chromophore exhibit a long lifetime corresponding to its ligand-localized triplet state ( 3 IL) evidenced from spectroscopic investigations and DFT calculations.
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ChemElectroChem
·
2021
·Vol. 8
·期 16
·3174-3180
·
IF 4.59
Yunxi Han,Shuaikang Zhu,Shuang Xu,Xiaopo Niu,Zhihong Xu,Rong Zhao,Qingfa Wang
Graphical The structural reconstruction of HKUST-1 on carbon fiber paper and the activity in CO 2 electroreduction is investigated. The HKUST-1 initially reconstructed into highly active 3D nanospheres and then into stable nanobelts after 120 minutes. The 3D nanospheres structure shows the best Faradaic efficiency of C 2 products up to 58.6 %. Metal-organic frameworks (MOFs) have been widely studied for electrochemical CO 2 reduction reaction (CO 2 RR). However, the application of negative potential tends to trigger its structural reconstruction and component alteration. It is of great significance to study the relationship between the structural evolution of MOF-derived materials and product selectivity under the reaction conditions. Herein, we fabricate a HKUST-1 thin film on carbon fiber paper by a facile electrodeposition approach to investigate the variation of CO 2 RR activity with HKUST-1 structural reconstruction. During the CO 2 RR process, the HKUST-1 reconstructs into two structures successively over time: 3D nanospheres composed of numerous small fragments and 3D nano-network composed of cross-linked nanobelts in different directions. The former shows a better catalytic activity due to more active sites, lower charge transfer resistance and higher Cu + /Cu 0 ratio. The optimum Faradaic efficiency (FE) of C 2 products (ethylene and ethanol) reaches 58.6 % at −0.98 V versus reversible hydrogen electrode (RHE).
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