APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Ke Ye,Tianfu Liu,Yanpeng Song,Qi Wang,Guoxiong Wang
Electrochemical CO 2 reduction reaction (CO 2 RR) offers an appealing route to simultaneously store intermittent renewable energy as value-added chemicals and close carbon cycle. Silver (Ag) catalyst is a promising candidate for the electrochemical conversion of CO 2 to CO, but the electrocatalytic properties are still insufficient for practical applications. Herein, we put forward a strategy to in situ reconstruct a heterogeneous Ag 2 S/Ag interface structure, in which their strong interactions facilitate CO 2 RR performance. The in situ reconstructive Ag 2 S/Ag catalyst achieves a large current density of 421.7 ± 14.4 mA cm –2 at –0.70 V vs . reversible hydrogen electrode (RHE) and maintains steadily at a current density of 244.5 ± 31.8 mA cm –2 and CO Faradaic efficiency of 99.1 ± 0.8 % at –0.49 V vs . RHE for 50 h, superior to state-of-the-art CO-selective Ag-based catalysts. Density functional theory calculations reveal that the in situ reconstructive Ag 2 S/Ag interface active sites stabilize the *COOH intermediate during CO 2 RR process.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jun Mou,Xingqi Fan,Fei Liu,Xiaodan Wang,Tianxiang Zhao,Peng Chen,Ziwei Li,Chunliang Yang,Jianxin Cao
The direct conversion of CO 2 hydrogenation to lower olefins via methanol as an intermediate is of great significance, but challenges still remain. Herein, we present a binary Mn 2 O 3 -ZnO oxide, which is responsible for catalytic hydrogenation of CO 2 to methanol. After combination of Mn 2 O 3 -ZnO and SAPO-34 molecular sieve, the catalytic reaction displays a markable increase. CO 2 adsorption by alkaline nature, followed by oxygen vacancy activation and synergistic hydrogenation over the binary Mn 2 O 3 -ZnO oxide are the prerequisites for the tandem reaction. However, the tandem spacing between oxide and molecular sieve plays a crucial role, because the suitable intimacy can induce enhanced methanol formation as intermediate via tandem dynamics effect, causing an apparent limitation for reverse water gas shift reaction at high temperature. The optimum mass ratio of 3:1 for two phases demonstrates that more components of binary oxide are needed to improve the rate of CO 2 hydrogenation to methanol, aiming to balance the two-step tandem reaction. Finally, under conditions of 380 ℃, 3 MPa and 3600 mL/g cat /h, 20%Mn 2 O 3 -ZnO/SAPO-34 tandem catalyst is obtained by physical ball milling after 15 min, with excellent stability, sulfur tolerance and catalytic performance with CO 2 conversion at almost 30%, lower olefins selectivity of 80.2% (propylene/ethylene = 5.6:1), and single-pass yield of 10.7%.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Nanhui Li,Ping Yan,Yuanhao Tang,Jianghao Wang,Xin-Yao Yu,Hao Bin Wu
Electrochemical reduction of carbon dioxide provides a feasible solution to the energy and climate crisis. Bi-based catalysts are promising candidates to electrochemically convert carbon dioxide (CO 2 ) into formic acid or formate. Herein, ligand-stabilized Bi nanosheets are obtained from in-situ electrochemical reduction of a Bi-based metal-organic framework, which exhibit remarkable electrocatalytic performance for CO 2 reduction. A high Faradic efficiency of 98 % for formate is achieved at a potential of -0.80 V vs . reversible hydrogen electrode (RHE) with an improved durability over 40 h. The remarkable electrocatalytic activity and stability could be attributed to the in-situ generated catalyst with abundant under-coordinated Bi active sites, which are effectively stabilized by residual ligands adsorbed on surface. This study demonstrates that ligand-stabilized under-coordinated surface sites would be facilely generated from in-situ transformation of metal-organic precursors for highly efficient CO 2 conversion.
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Journal of CO2 Utilization
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2021
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IF 7.132
Jinsong Shi,Hongmin Cui,Jianguo Xu,Nanfu Yan,Chao Zhang,Shengyong You
Porous carbon with specifically designed structure as CO 2 adsorbent is a very attractive and interesting research topic. In this study, we presented the synthesis and CO 2 adsorption of flower shaped porous carbons. Flower-like hydrochar derived from the hydrothermal reaction of glucose, cobalt sulfate, and hexamethylenetetramine was used as the precursor, which was converted to carbon flower during CO 2 activation. The flowers had hierarchically macro-meso-microporous structure. Interspaces and voids were formed by assembly of the petals, and the petals were distributed with pores of different scales. The formation mechanism of, and influences of various synthesis parameters on the flower shape were studied and analyzed. The carbon flowers exhibited surface area of 422−691 m 2 /g, and very high nitrogen content of 9.31–11.91 wt%. CO 2 adsorption performances of the carbon flowers were also studied. Influences of the textural properties and doped nitrogen on the adsorption performances were investigated. The experiment results demonstrated that nitrogen doping showed positive effects on CO 2 uptake at 1 bar, and had strong influence on the CO 2 /N 2 selectivity.
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ACS Applied Energy Materials
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2020
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IF 4.473
Zhongkai Xie,Yuyan Xu,Di Li,Suci Meng,Min Chen,Deli Jiang
The highly efficient spatial carrier separation and abundant active sites are significant for CO2 photocatalytic reduction efficiency. Herein, an ultrathin Bi2O3 nanosheet/Bi2WO6 network heterostructure is successfully synthesized via a covalently bonded epitaxial growth strategy. Due to cosharing of the Bi–O tetrahedron between Bi2O3 and Bi2WO6, this heterostructure exhibits a compact interface, which can provide a highway for the charge transfer and then boost their separation. Moreover, the pores generated from the hierarchical structure afford abundant exposed photocatalytic active sites. Thus, the optimal Bi2O3/Bi2WO6 heterostructure (BOBWO-12) shows superior photocatalytic performance for CO2 reduction with an ultrahigh selectivity as well as the removal of RhB. Notably, the photocatalytic CO generation rate over BOBWO-12 reaches up to 17.39 μmol·g–1·h–1, which is 18.0 and 4.2 times higher than that of bulk-Bi2WO6 and Bi2WO6 nanosheets, respectively, and the selectivity is of about 95.4%. Moreover, the Bi2O3/Bi2WO6 heterostructure also exhibits improved long-term stability, resulting from the firm heterointerface. Our studies present a conventient avenue to construct a high-efficiency heterostructure photocatalyst with a firm interface by the covalently bonded epitaxial growth method for CO2 reduction.
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RSC Advances
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2021
·Vol. 11
·期 4
·2040-2046
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IF 3.361
Yang Liu,Xin Liang,Jie Zhang,Jimmy Yun,Zuobo Yang
In this study, monodispersed NiRu nanocrystals with a diameter of 3 nm were synthesized at 90 °C via a tuning hot-inject method to lower the temperature of the organic phase synthesis of monodispersed nanomaterials. The key factor for the nanocrystalline formation of NiRu alloy nanocrystals was summarized in detail. Simultaneously, the synergistic effect of Ni and Ru in CO2 methanation was explored. Doping trace Ru can significantly improve the conversion rate of CO2 methanation and CH4 selectivity. The underlying mechanism was studied in detail via X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature-programmed hydrogen reduction (H2-TPR) and desorption (H2-TPD) tests, and temperature-programmed desorption of CO2 (CO2-TPD). This study gives out a new way for the general synthesis of monodisperse nickel-based nanocrystals and provides a reference for the development and application of monodispersed nanoparticles for CO2 methanation.
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ACS Catalysis
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2021
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IF 13.084
Tian-Wen Jiang,Ya-Wei Zhou,Xian-Yin Ma,Xianxian Qin,Hong Li,Chen Ding,Bei Jiang,Kun Jiang,Wen-Bin Cai
The electrochemical CO2 reduction reaction (CO2RR) on Pd-based electrodes to dissolved formate and/or gaseous CO is largely dependent on potential and the electrode material, yet there is a lack of molecular-level insights into this dependence. Herein, in situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) in conjunction with differential electrochemical mass spectrometry (DEMS), gas chromatography (GC), and nuclear magnetic resonance (NMR) measurements is applied to investigate the CO2RR on Pd and Pd-B film electrodes, providing a direct observation of the role of surface CO as well as the B-doping effect at varied potentials. Comprehensive spectrometric results reveal that at lower overpotentials, CO gradually accumulates on both Pd electrode surfaces poisoning the dominant formate pathway, while at higher overpotentials, surface CO forms facilely with linearly bonded CO (the minor surface CO species) acting as an active precursor and bridge-bonded CO (the major surface CO species) as a spectator toward the gaseous CO product. Moreover, B-doping in Pd hinders CO formation and promotes formate production on the Pd-B electrode for the CO2RR as compared to that on the pristine Pd electrode at all of the overpotentials under investigation.
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JOURNAL OF POWER SOURCES
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2021
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IF 9.127
Youxu Yu,Fengjia Xie,Rong Chen,Xun Zhu,Qiang Liao,Dingding Ye,Jinwang Li,Sihong Song
The objective of this work is to explore the role of CO 2 in the photocatalytic fuel cell with TiO 2 as the photoanode and methanol as a fuel under acid condition by making the anode electrolyte saturated with CO 2 . It is interesting to find that the performance of the photocatalytic fuel cell can be improved at low methanol concentration in the presence of CO 2 . This is probably because TiO 2 has an adequate conduction band for photocatalytic reduction of CO 2 to organics at the photoanode, which increases the methanol concentration at the catalytic surface to alleviate the mass transfer issue encountered in the low methanol concentration operation, and hinders the recombination of the electron-hole pairs. Moreover, the methanol concentration at the outlet of the photoanode can be even higher than the supplied methanol concentration. However, this effect is weakened and even disappears as the supplied methanol concentration increases. This work gives new insights into the role of CO 2 in the photocatalytic fuel cell with the photoanode having an adequate conduction band for photocatalytic reduction of CO 2 .
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REACTIVE & FUNCTIONAL POLYMERS
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2021
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IF 3.975
Hui Wang,Yunxia Ni,Zhiyue Dong,Qiang Zhao
Interface compatibility is crucial to performance and robustness of nanocomposite membranes for molecular separation. In this work, a covalent crosslinking method was exploited to fabricate polydimethylsiloxane/metal-organic-frameworks (PDMS/MOFs) mixed matrix membranes with improved interfacial compatibility. Zirconium MOF particles (UiO-66-NH 2 ) were grafted with methoxysilane groups, which further formed covalent crosslinks with silanol terminated PDMS matrix. The strengthened interfacial compatibility prevented sedimentation and aggregation of MOF particles in PDMS precursor solution during the solvent evaporation process, thus the composites showed good membrane formation ability at high MOFs loading (60 wt%). Tensile strength of the hybrid membrane is 2.8 times improved while retaining good flexibility. Moreover, the CO 2 /N 2 selectivity and CO 2 permeability of the PDMS composite membrane incorporated with 40 wt% UiO-66-MS particles are improved by 1.3 times and 0.7 times, respectively.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Tianjiao Wang,Hongyan Yao,Ningning Song,Yanchao Yang,Kaixiang Shi,Shaowei Guan
In recent years, linear polyimides of intrinsic microporosity have been widely used in the field of gas adsorption and separation because of their high BET surface area and microporous structures. Most of the microporous structures come from the twisted main-chain structures in the linear polyimides of intrinsic microporosity. Therefore, most linear polyimides (PI) without twisted structure have no porosity. Herein, to construct the linear polyimide with microporous structure, a sequence of microporous polyimides (PIs-CL) were constructed from the flexible linear polyimide precursors through the thermal crosslinking reaction. The polyimide precursors without twisted structure were synthesized from a well-designed diamine TFVBPA with cross-linkable ethynyl groups and several commercial dianhydrides (ODPA, BPDA, PMDA and 6FDA) by polycondensation to research the influence of the main-chain structure on the porous characters. The introduction of crosslinked structures gives the linear crosslinked polyimides (PIs-CL) with porous structures. The PIs-CL show obviously improved porosity (0.52–1.71 nm) and higher BET surface area (337–618 m 2 g −1 ) than those of the uncrosslinked polyimides (PIs). Moreover, PIs-CL have favorable CO 2 adsorption (5.7–9.3 wt%) as well as good CO 2 /N 2 selectivity (34.4–58.5) at 273 K, which are better than other polyimides materials. The introduction of crosslinked structures is an effective way to improve microporous porosity and gas sorption performance.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Sizhu Ren,Ziyuan Wang,Muhammad Bilal,Yuxiao Feng,Yunhong Jiang,Shiru Jia,Jiandong Cui
Multienzymatic conversion of carbon dioxide (CO 2 ) into chemicals has been extensively studied. However, regeneration and reuse of co-factor are still the main problems for the efficient conversion of CO 2 . In this study, a nanoscale multienzyme reactor was constructed by encapsulating simultaneously carbonic anhydrase (CA), formate dehydrogenase (FateDH), co-factor (NADH), and glutamate dehydrogenases (GDH) into ZIF-8. In the multienzyme reactors, cationic polyelectrolyte (polyethyleneimine, PEI) was doped in the ZIF-8 by dissolving it in the precursors of ZIF-8. Co-factor (NADH) was anchored in ZIF-8 by ion exchange between PEI (positive charge) and co-factor (negative charge), and regenerated through GDH embedded in the ZIF-8, thus keeping high activity of FateDH. Activity recovery of FateDH in the multienzyme reactors reached 50%. Furthermore, the dissolution of CO 2 in the reaction solution was increased significantly by the combination of CA and ZIF-8. As a result, the nanoscale multienzyme reactor exhibited superior capacity for conversion of CO 2 to formate. Compared with free multienzyme system, formate yield was increased 4.6-fold by using the nanoscale multienzyme reactor. Furthermore, the nanoscale multienzyme reactor still retained 50% of its original productivity after 8 cycles, indicating excellent reusability.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Li Ma,Yu Qiu,Min Li,Dongxu Cui,Shuai Zhang,Dewang Zeng,Rui Xiao
Reverse water gas shift on the basis of chemical looping technology provides a viable method for efficiently converting CO2 to CO for hydrocarbons at moderate temperature (<750 °C). However, the commonly available oxygen carrier materials are insufficiently active because of the degrading effect at relatively low temperatures. In this paper, we present several Co, Mn codoped ferrites in search of oxygen carrier materials as highly active redox materials for a midtemperature chemical looping CO2 splitting process. The results show that up to ∼142.3 μmol·g–1·min–1 of CO production rate and ∼8.8 mmol·g–1 of CO yield are achieved by Mn0.2Co0.8Fe2O4 at 650 °C. The production rate and yield of CO of the codoped ferrites during the CO2 splitting process are comparable to those of the state-of-the-art perovskites which commonly contain rare-metal elements.
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