CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2022
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IF 0.847
Wei-Feng YOU,Xiao XU,Ai-Hui CAO,Zhi-Jie TAO,Long-Tian KANG
The electrocatalysts containing cobalt-pyrrolic nitrogen-carbon (Co-N 4 -C) moiety for CO 2 reduction reaction (CO 2 RR) have caught much attention. However, the effects of Co valence state and its synergy with graphene substrate are not clear yet. In this work, cobalt porphyrin (CoTPP) molecule with the intrinsic Co-N 4 -C moiety is successfully combined with graphene oxide (GO) via three kinds of liquid-phase methods. The ratio of CoTPP to GO and the valence state of Co atom are studied to explore their catalysis for CO 2 RR to CO. It is found that axially-coordinated Co(III)TPPCl/GO nanocomposites synthesized via a chemical method exhibit better ability for CO 2 RR, as compared with Co(II)TPP+GO and/or Co(III)TPPCl+GO nanocomposites obtained via a physically mixing way. After optimizing the ratio of CoTPP to GO, the Faradaic efficiency (FE) is more than 90% for CO 2 RR to CO between –0.7 and –0.8 V vs . reversible hydrogen electrode (RHE) in Co(III)TPPCl/GO75. The synergy between CoTPP and GO and the effect of Co valence state are systematically investigated, indicating that their strong interaction plays the key role in electrocatalytic CO 2 RR.
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高影响因子
ENERGY
·
2022
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IF 8.857
Xiangyu Li,Zhiqing Wang,Zheyu Liu,Ru Feng,Shuangshuang Song,Jiejie Huang,Yitian Fang
A “wet gel impregnation” method (WGI) was applied to prepare modified CO 2 sorbents derived from alumina-extracted residue of coal ash (AR). Tetraethylene pentamine (TEPA) was selected as an amine polymer and it was evenly dispersed on the surface of AR. And the effects of loading amount, impregnation method, and adsorption temperature on CO 2 adsorption capacity of the sorbent were investigated by thermogravimetric analyzer (TGA). The results showed that the desired sorbent with 60% TEPA loading via WGI had the maximum CO 2 adsorption capacity of 3.45 mmol/g under 100% CO 2 at 75 °C. This was attributed to the fact that the loading in wet gel state dramatically improved TEPA dispersion on the supports and increased the saturated loading of amine. Moreover, the sorbent still maintained stable CO 2 uptake after five repeated adsorption-desorption cycles. These results suggested that amine-impregnated AR sorbent synthesized by WGI was an excellent and low-cost sorbent for CO 2 capture.
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Energy & Environmental Materials
·
2022
·Vol. 6
·期 3
·e12364
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IF 13.443
Liang Lu,Chunwen Sun,Jian Hao,Zelin Wang,Sergio F. Mayer,Maria Teresa Fernández-Díaz,José Antonio Alonso,Bingsuo Zou
The recovery and utilization of carbon dioxide (CO 2 ) is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality. The Na-CO 2 battery made with cheap alkali metal sodium and greenhouse gas CO 2 is an effective strategy to consume CO 2 and store clean renewable energy. However, the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO 2 batteries. In this work, magnesium-doped Na 3 Zr 2 Si 2 PO 12 (NZSP) was studied as a solid electrolyte for solid-state Na-CO 2 batteries. The ionic conductivity of Na 3.2 Zr 1.9 Mg 0.1 Si 2 PO 12 reaches 1.16 mS cm −1 at room temperature by replacing Zr ions in Na 3 Zr 2 Si 2 PO 12 with Mg ions, and the structural changes are analyzed by neutron powder diffraction. The composite electrolyte consisting of highly conductive Na 3.2 Zr 1.9 Mg 0.1 Si 2 PO 12 and high processability poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) is utilized for the first time to assemble a solid-state Na-CO 2 battery. The cell shows a full discharge capacity of 7720 mAh g −1 at 200 mA g −1 . The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g −1 and at a cut-off capacity of 500 mAh g −1 . This work demonstrates a promising strategy to design high-performance solid-state Na-CO 2 batteries.
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ENERGY & FUELS
·
2022
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IF 4.654
Zhijun Zhao,Jubao Gao,Mingsheng Luo,Xinyue Liu,Yongsheng Zhao,Weiyang Fei
In recent decades, ionic liquids (ILs) have been developed as an ideal and reversible decarbonization solvent. However, some pitfalls, such as the low CO2 capacity and high viscosity of ILs, limit their further scale up and industrial application. Therefore, in this work, three novel functional ILs [N8881][NIA], [N8881][For], and [N8881][Ac] were synthesized after using a molecular design method to capture CO2 at 303.15–333.15 K and pressures up to 1000 kPa. The experimental results illustrate that [N8881][NIA] presents the smallest viscosity and the highest CO2 solubility. The capacity order is [N8881][NIA] > [N8881][For] > [N8881][Ac] under the same experimental conditions. The CO2 recyclability experiments using [N8881][NIA] show the stability of CO2 solubility after 5 cycles. The quantum chemistry simulations at the level of DFT/B3LYP with 6-311++G(d,p) basis sets were used to study the CO2 absorption mechanism in the studied ILs from the molecular viewpoint. Simulation results illustrated that the higher interaction energy between CO2 and ILs means more CO2 absorbed in these ILs, which agreed well with the experimental results. The atoms in molecules theory and the function of the reduced density gradient were also used to calculate the interactions in these IL–CO2 systems. Results show that the majority of these interactions present an electrostatic character.
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Biomass Conversion and Biorefinery
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2022
·Vol. 13
·期 15
·14049-14058
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IF 4.05
Yan Mi,Zhang Yan,Grisdanurak Nurak,Wibowo Haryo,Yu Caimeng,Kanchanatip Ekkachai
One outstanding advantage of supercritical water gasification (SCWG) coupled with CO 2 capture and storage (CCS) technology is to realize the conversion of bio-waste into hydrogen-rich syngas. In this study, metal organic frameworks of copper benzene-1,3,5-tricarboxylate (Cu-BTC) were synthesized via solvothermal method with different synthesis time and used as adsorbent for capturing CO 2 from SCWG model syngas. The effect of synthesis time, adsorption temperature, and adsorption pressure on CO 2 adsorption capacity of Cu-BTC was evaluated using analysis of variance (ANOVA). The Pareto chart showed that adsorption pressure had significant effect on CO 2 adsorption capacity, and the surface plot indicated that CO 2 adsorption capacity increased with higher adsorption pressure and lower adsorption temperature. Cu-BTC with 48-h synthesis time had the largest specific surface area (1737 cm 2 /g) and pore volume (0.73 cm 3 /g), and it exhibited the highest CO 2 capacity of 19.83 mmol/g and 13.56 mmol/g at 0 °C and 25 °C, respectively. The adsorption results showed that CO 2 concentration in multi-component gas decreased from 48.75 to 12.9%, and H 2 concentration increased from 38.75 to 75.45%. Therefore, Cu-BTC has the potential for removal of CO 2 from SCWG syngas, and more work is necessary to further improve the adsorption capacity and selectivity. Graphical abstract
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CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Linlin Wang,Xin Li,Leiduan Hao,Song Hong,Alex W. Robertson,Zhenyu Sun
To facilitate the electrochemical CO 2 reduction (ECR) to fuels and valuable chemicals, the development of active, low cost, and selective catalysts is crucial. We report a novel ECR catalyst consisting of CuO nanoparticles with sizes ranging from 1.4 to 3.3 nm anchored on Cu metal-organic framework (Cu-MOF) nanosheets obtained through a one-step facile solvothermal method. The nanocomposites provide multiple sites for efficient ambient ECR, delivering an average C 2 H 4 faradaic efficiency (FE) of ~50.0% at –1.1 V (referred to the reversible hydrogen electrode) in 0.1 mol/L aqueous KHCO 3 using a two-compartment cell, in stark contrast to a C 2 H 4 FE of 25.5% and 37.6% over individual CuO and Cu-MOF respectively, also surpassing most newly reported Cu-based materials under similar cathodic voltages. The C 2 H 4 FE remains at over 45.0% even after 10.0 h of successive polarization. Also, a ~7.0 mA cm −2 C 2 H 4 partial geometric current density and 27.7% half-cell C 2 H 4 power conversion efficiency are achieved. The good electrocatalytic performance can be attributed to the interface between CuO and Cu-MOF, with accessible metallic moieties and the unique two-dimensional structure of the Cu-MOF enhancing the adsorption and activation of CO 2 molecules. This finding offers a simple avenue to upgrading CO 2 to value-added hydrocarbons by rational design of MOF-based composites.
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ACS Catalysis
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2022
·
IF 13.7
Shuangxi Lin,Qiang Wang,Maoshuai Li,Ziwen Hao,Yutong Pan,Xiaoyu Han,Xiao Chang,Shouying Huang,Zhenhua Li,Xinbin Ma
Controlling the selectivity of CO2 hydrogenation by catalysis is a fundamental challenge. This study examines the interrelation between active sites and reaction pathways in Ni-catalyzed CO2 hydrogenation. The alloying of Ni with Zn to charged (Niσ––Znσ+) active sites modifies the electronic structure and d-band center, weakens the interaction with CO/H2, and preferentially catalyzes the reverse water gas shift to CO with the thermodynamically favored methanation pathway switched off. The charged dual sites can stabilize the activated CO2 species in a η2(C, O) bridge configuration, directly dissociate the C═O bond to *CO, and promote CO desorption. The mechanistic investigation has elucidated the reaction pathways in the Ni-catalyzed CO2 hydrogenation and identified the crucial intermediates that impacted the product selectivity, which can provide a theoretical guide for the Ni-based catalyst design.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Minmin Gou,Ruili Guo,Hengheng Cao,Weifang Zhu,Fu Liu,Zhong Wei
Mixed matrix membranes (MMMs) for separating CO 2 /CH 4 mixture were prepared through incorporating Cu@Al(bpydc) into a Pebax polymer in which Cu@Al(bpydc) synthesized through a competitive coordination method achieved a controllable micro/mesopores structure and abundant functional sites for CO 2 . The hierarchical pores of Cu@Al(bpydc) provided multidimensional diffusion channels in the Pebax matrix, which increased the diffusion of CO 2 . In addition, the abundant chemical groups, such as the polar group COO – and nitrogen Lewis basic groups, created a microenvironment with multiple CO 2 affinity sites in the membrane, increasing the selectivity of CO 2 . A MMM loaded with 5 wt% Cu@Al(bpydc) exhibited excellent CO 2 separating property under wet mixed-gas test conditions. In particular, the CO 2 permeability and selectivity of the MMMs were increased by 92.90% and 27.10% respectively, compared with those of pure Pebax, showing exceptional potential for the separation and capture of CO 2 from biological natural gas.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Wenchao Zheng,Zuyi Yan,Rui Zhang,Wusan Jiang,Xiao Luo,Zhiwu Liang,Qi Yang,Hai Yu
The kinetics between BZA and CO 2 were investigated by the stopped-flow apparatus over the BZA concentration range from 0.05 to 0.1 mol/L (0.54–1.07 mass%), and over the temperature range from 293 to 313 K. The results also show that the predicted CO 2 absorption rate exhibits good agreement with the experimental data with an absolute average deviation (AAD) of 5.15% and 4.15% with respect to the zwitterion and termolecular models, respectively. Furthermore, the NMR experiments confirmed the formation of carbamates. The VLE plots were made with speciation data obtained from NMR techniques applied to the CO 2 -BZA-H 2 O system with CO 2 loading of 0–0.67 mol CO 2 /mol BZA at 298 K. A new VLE model was proposed, and the predicted results exhibit good agreement with the experimentaly measured results.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Chengyuan Duan,Meili Ding,Yi Feng,Mengjue Cao,Jianfeng Yao
Integration of Lewis acid and base sites and oxygen surface groups in one catalyst is favorable to promote CO 2 cycloaddition reaction. Here, Zn-ZIF-L was used as starting material to design one kind of catalyst with multiple active sites via pyrolysis and oxidization treatment. The well-dispersed ZnO nanoparticles and pyridinic nitrogen in nitrogen-doped carbon serve as Lewis acid and base sites to activate epoxide and CO 2 while oxygen surface groups help promote the ring-opening reaction of epoxides. Results show that Zn-ZIF-L derived catalyst displays high catalytic activities for CO 2 cycloaddition (6 h, 83% of yield) under mild conditions (70 °C and 0.1 MPa CO 2 ) and outperforms ZIF-8 derived catalyst. Moreover, the obtained catalyst also achieves a satisfactory photothermal catalysis of cycloaddition reaction under light irradiation (120 mW/cm 2 ), which makes our sample a promising catalyst for CO 2 conversion.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Zhen-Yu Chen,Qin-Long Hong,Hai-Xia Zhang,Jian Zhang
Improving the stability and charge transportation efficiency of lead halide perovskites is the key for their practical photocatalytic applications. Herein, we designed and synthesized a microporous boron imidazolate framework (BIF-122-Co) by cross-linking boron imidazolate ligands and benzene carboxylate with metal ions, which was further used as a host matrix to encapsulate CsPbBr3 perovskite via a sequential deposition route to obtain a composite material, CsPbBr3/BIF-122-Co. Due to the intimate host–guest interfacial contact in the composite material, BIF-122-Co not only provided a physical protective barrier for CsPbBr3 but also accelerated the photoinduced charge separation process in the photocatalytic CO2 reduction reaction. The work provided a guide for exploration of excellent perovskite/metal–organic framework (MOF) composites.
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高影响因子
FUEL
·
2023
·
IF 7.4
Cong Luo,Houfang Lu,Haoru Tang,Kejing Wu,Yingying Liu,Yingming Zhu,Siyang Tang,Binshen Wang,Bin Liang
The chemical conversion of inert carbon dioxide (CO 2 ) into high value-added chemicals is a continuing challenge. In this work, an experimental and theoretical mechanism study is presented for one-pot synthesis of glycerol carbonate (GC) from CO 2 , glycerol (Gly), and propylene epoxide (PO) catalyzed by 1,8-diazabicyclo[5.4.0]undec-7-enenium iodide (HDBUI) ionic liquid. 92% GC yield was obtained in the one-pot reaction through cycloaddition of CO 2 with PO to produce propylene carbonate (PC), followed by transesterification of Gly with PC to yield targeted products. Density functional theory (DFT) calculations were used to unveil the HDBUI-mediated catalytic mechanism and key catalytic species. It was revealed that the HDBUI-catalyzed cycloaddition was assisted by the hydrogen bond donor Gly, the transesterification reactant, by promoting the ring-opening of PO and the insertion of CO 2 . By activating Gly hydroxyl group, alkaline HDBUI-bonded propan-1-ylium-2-yl carbonate, an intermediate in cycloaddition, catalyzed transesterification. The complementary mechanism of cycloaddition and transesterification in the one-pot provides a feasible method for utilizing inert CO 2 .
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