iScience
·
2024
·
IF 4.6
Binxia Yuan,Yuhao Liu,Hong Qian,Rui Zhu,Chengxi Zhang,Weiling Luan
In this study, the theoretical calculations proves that the combination of oxygen vacancy and amorphous carbon films in TiO 2 (V O -CT) can effectively reduce the energy bandgap and work function. The minimum Gibbs free energies required for the CO 2 RR reaction of V O -CT are 0.20 eV, which is lower than pure TiO 2 . The amorphous c@TiO 2 nanomaterials with oxygen vacancy and mesoporous structures (V O -MCT) are prepared with the P123 surfactant as the template and oxalic acid as an inducer. The electron paramagnetic resonance indicates the presence of abundant oxygen vacancy defects in the samples. UV-vis spectra indicate that the mesoporous structure enhances light absorption capacity. The photocatalytic CO 2 reduction tests show that the highest conversion rates for CH 4 and CO of V O -MCT are 14 μmol g −1 h −1 and 10.66 μmol g −1 h −1 , respectively. The electron consumption rate of V O -MCT is 12.43 times higher than that of commercial TiO 2 (P200).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Meisi Chen,Yin Tong,Weida Chen,Tong Lei,Xinbao Zhu,Bo Fu,Feng Zhang,Youting Wu
This study introduces innovative hydrophobic nanostructured composite deep eutectic solvents (HS-SiO 2 /DBU-EG) to overcome limitations of amine absorbents in humid CO 2 . The HS-SiO 2 /DBU-EG achieved a significantly enhanced CO 2 absorption capacity of 4.14 mol/kg and maintaining a high regeneration efficiency of 95 %, attributed to its inherent synergistically hydrophobic nanostructure. In contrast, while DBU-EG showed improved absorption under humid CO 2 but reduced regeneration performance. Spectroscopic analysis revealed that DBU-EG relies on hydrolysis-induced N-sites for absorption, but the resulting products are challenging to decompose. Conversely, HS-SiO 2 /DBU-EG utilizes the O-sites of EG as the absorption sites, a mechanism supported by thermodynamic analysis and quantum calculations demonstrating a low enthalpy change value of the reaction. Fixed-bed experiments further confirmed its efficient and continuous absorption performance. This research emphasizes the value of low-energy absorption mechanisms and hydrophobic design for advanced industrial CO 2 capture.
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JOURNAL OF POLYMER RESEARCH
·
2024
·Vol. 31
·期 5
·1-14
·
IF 2.6
Zhang Shoucun,Bian Yujing,Yang Chun
A new strategy was developed to build a CO 2 -philic/hydrophilic surfactant by combining the common free radical polymerization and the grafting modification technology, and a brush polymer was synthesized with poly(vinyl acetate)(PVAc) based copolymer as the CO 2 -philic group (as the main chain) and the methoxy poly(ethylene glycol) (mPEG) as the hydrophilic part (as the branched chain) (PVAc- g -mPEG). The CO 2 -philic ability can be controlled by adjusting the chain length of the CO 2 -philic fragment. The results indicate that PVAc- g -mPEG has excellent surfactant activity, and can emulsify the CO 2 /H 2 O system to obtain the CO 2 -in-water (C/W) high interval phase emulsion (HIPE 80%, v/v), which can remain stable for more than 20 h. If using the monomers/crosslinking agent solution instead of water, the highly porous monolithic materials will be obtained after the continuous phase is polymerized. In this paper, polyacrylamide (PAM) and poly(acrylamide/diethyl aminoethyl methacrylate) (PADM)-based porous monolithic materials were prepared. These materials were used to remove bovine serum albumin (BSA, as the model matter) from the solution, and the results indicated that PAM-based porous monolithic materials had almost no enrichment capacity for protein, while PADM-based porous monolithic materials can adsorb BSA up to 129.3 mg/g.
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FUEL
·
2024
·
IF 6.7
Mengmeng Zhang,Xu Chen,Hui Xue,Zhijia Zhang,Yang Wang,Yifang Zhang,Yida Deng,Yong Jiang
As an effective strategy to turn waste into treasure, electrochemical CO 2 reduction reaction (eCO 2 RR) producing value-added chemicals such as HCOOH attracts unremitting interest. However, the practical applications are limited by poor activity and selectivity, the key is to develop economical-efficient catalysts. Herein, gradient-doped Sn on the CuO surface (Sn-CuO) was developed for eCO 2 RR in an H-cell. Typically, the main reaction pathway of *OCHO → HCOOH was obtained via in situ experiments and further verified by theoretical calculations. Furthermore, the lowest Δ G *OCHO and Δ G *OCHO − Δ G *H as well as the highest Δ G *COOH enlist Sn-CuO with sufficient proton to produce HCOOH while inhibiting CO and H 2 by-products. Finally, the synthesized Sn-CuO delivers a maximum partial current density (23.6 mA cm −2 ) at −1.3 V REH and Faradic efficiency (91.5 %) at −1.2 V RHE for HCOOH, indicating excellent activity and selectivity.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuan Wang,Guomin Xu,Chao Xue,Changming Zhang,Jinbo Xue,Xiaochao Zhang
It is rather important to develop an efficient, stable and economical photocatalyst for solar-driven CO 2 reduction. Herein, N-doped hierarchical porous carbon spheres (NPCS-F6) with metal-like activity is synthesized using acrylamide and F127 as nitrogen source and soft template, and the effective synergy between nitrogen-containing species and hierarchical pore structure makes the samples exhibit excellent CO 2 reduction properties. XPS characterization illustrates that the introduced pyridine nitrogen and pyrrole nitrogen groups contribute to the increase of CO 2 reduction sites on the surface of the material. N 2 adsorption analysis verifies the existence of hierarchical pore structures in which micropores facilitate the exposure of more adsorption active sites, while mesopores and macropores can be used as transfer channels to connect the internal micropores and reduce the molecular diffusion resistance to improve CO 2 adsorption performance. In addition, the pore structure of the samples prepared with P123 and CTAB as templates is mainly microporous, whereas carbon spheres with hierarchical pores coexisting are obtained with F127 as template. The evaluation of photocatalytic CO 2 reduction activity shows that the CO yield of NPCS-F6 could reach 17.56 μmol·g −1 for 8 h, which is 1.17 times, 1.08 times and 1.07 times of the original NCS-8 (15.05 μmol·g −1 ), NPCS-P6 (P123 as soft template, 16.25 μmol·g −1 ) and NPCS-C1 (CATB as soft template, 16.39 μmol·g −1 ), respectively. Comprehensive characterization results are analyzed to propose a possible mechanism for photocatalytic CO 2 reduction, in which photogenerated electron-hole pairs are generated inside the material under light conditions, and the photogenerated electrons are transferred to the N-6/N-5 active sites through the electron transfer channel N-Q to react with CO 2 molecules adsorbed on the surface to be reduced to CO. Finally, our results provide a favorable and feasible strategy to synthesize metal-free photocatalysts for high-efficiency CO 2 adsorption and targeted reduction of CO 2 to CO.
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FUEL
·
2024
·
IF 6.7
Changming Zhang,Yuan Wang,Xiaochao Zhang,Zhiyan Dong,Wensheng Wu,Caimei Fan
It is rather essential to increase CO 2 adsorption and improve separation efficiency of photoinduced carriers by solar-driven CO 2 reduction. Herein, we proposed a facile approach to synthesize millimeter-sized polyacrylonitrile-based carbon spheres (PANACSs) as a bifunctional adsorbent and self-nitrogen-doped source under a mild condition, and then embeds the highly active CeO 2 to construct a CeO 2 @PANACSs composite with strong adsorption capacity and high reduction activity. The involved XRD, XPS, SEM, N 2 adsorption/desorption, CO 2 adsorption, UV–vis DRS, EIS, PL and In situ FTIR spectra were characterized. Results suggested that the obtained PANACSs can act as a catalyst to drive the reduction of CO 2 into CO under visible light irradiation. CeO 2 @PANACSs showed the highest performance of photocatalytic reduction of CO 2 for 10 h (210.65 μmol·g −1 ), and the yield of CO evolution is approximately 1.83 times and 17.42 times higher than that of pristine CeO 2 and PANACSs, respectively. We found that the existence of nitrogen-containing functional groups further promoted the adsorption and activation of CO 2 . Among them, pyridinic nitrogen and pyrrolic nitrogen can be used as adsorption and activation sites to accelerate the separation and transfer of e - -h + . Furthermore, Ce 4+ on the surface of CeO 2 acts as an electron capture agent, which captures the electrons that are not transferred in time and reduces itself to Ce 3+ , and then the formed Ce 3+ reduces the adsorbed CO 2 to CO. Finally, the possible mechanism is proposed to depict the photocatalytic CO 2 reduction over the CeO 2 @PANACSs. Our finding provides a noteworthy promising strategy to construct bifunctional composite photocatalysts for achieving the high-efficient CO 2 adsorption and photoreduction to CO.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jie Zhu,Sifan Wang,Jiaji Zhang,Zhecheng Fang,Weitao Ji,Gaobo Lin,Lei Guo,Bolong Li,Jianghao Wang,Jie Fu
Constructing a stable Cu 0 /Cu 2+ interface is critical for enhancing the C-C coupling during the process of CO 2 electroreduction. However, the high-valence Cu species are unstable under the operating conditions. Herein, polyhedral-shaped CuO is coated with hydroxy-rich SiO 2 nanoparticles (m-SiO 2 /CuO) to stabilize the Cu 2+ species, enabling efficient CO 2 reduction to the ethylene product. Significantly, the optimal m-SiO 2 /CuO catalyst exhibits an impressive Faradaic efficiency of 55.5 % and an industrial-level partial current density of 500 mA cm −2 toward ethylene. Fourier transform infrared spectra and X-ray photoelectron spectra reveal that the strong interfacial interaction between CuO and hydroxy-rich SiO 2 is conducive to stabilizing the Cu 2+ species. In-situ characterizations reveal that the Cu 0 /Cu 2+ interface facilitates CO 2 activation and the key intermediate *OCCHO, thus promoting the production of ethylene. This work paves the way for developing advanced electro-catalysts of producing ethylene.
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Catalysts
·
2024
·Vol. 14
·期 10
·707
·
IF 3.8
Zengjing Guo,Shuguang Ning,Shicheng Xu,Yongying Zhang,Yifan Dong,Hongjing Han
Ambient condition-determined chemical CO2fixation affords great promise for remitting the pressure of CO2release. The construction of a microporous environment easily captures CO2molecules around the reactive sites of the catalyst to reinforce the reaction process. Herein, multi-hydroxyl-containing hyper-crosslinked organic polymers (HCPs-OH-n) are synthesized by the polymerization of 1,4-dichlorobenzyl (DCX) andm-trihydroxybenzene in the monosaccharide form in a Friedel–Crafts alkylation hypercrosslinking process (FCAHP). By tuning the DCX ratio in the FCAHP, the structural properties can be regulated to create a more microporous surface in the HCPs-OH-n; meanwhile, the formed multi-hydroxyl species in the microporous environment could induce the easy interaction between hydroxyls and epoxides by forming a hydrogen bond, which improves the activation of epoxides during the cycloaddition reaction to synthesize the cyclic carbonates at ambient conditions. The structural properties suggest that HCPs-OH-npossess a large surface area with appreciable microporous and mesoporous distribution. As expected, the HCPs-OH-3 bearing the most abundant mesoporosity affords the highest reactivity in the chemical CO2fixation to cyclic carbonates and is endowed with rational recoverability.
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iScience
·
2024
·
IF 4.6
Rui Yang,Wanbin Lin,Yunjuan He,Manish Singh,Liangdong Fan
Solid oxide electrolysis cells hold unique Faraday efficiency and favored thermodynamic/kinetics for CO 2 reduction to CO. Perovskite oxide–based composite materials are promising alternatives to Ni-based cermet electrodes in SOECs. However, contrary results of the electrocatalytic activity over single-phase perovskite oxide exist and the rationale of the negative effect is not well revealed. In this work, two-phase perovskite materials with various complementary properties and unique interfaces are self-assembled, which was realized by “subtractive” defect-driven phase separation. The obtained heterostructure electrodes showed reduced performance over that of single-phase materials although the cyclic stability was improved. The main reasons for the performance degradation are the decrease of electrical conductivity, oxygen vacancy concentration while increasing the average valence state of B-site Fe cations, and electrode surface Sr aggregation. This work highlights the self-assembly method and insight into the rational design and synthesis of active electrodes/catalysts for CO 2 conversion in solid oxide cells.
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Molecular Catalysis
·
2025
·
IF 4.9
Jun Ma,Shiyan Li,Bing Xu,Wei Chu,Qian Jiang,Yuefeng Liu
Converting CO 2 from the coal chemical industry into natural gas via methanation reaction, coupled with green hydrogen, is a promising strategy for reducing carbon emissions. While Ni-based catalysts are cost-effective and widely used for CO 2 methanation, their performance is often hindered by low temperatures activity. We confined LaO x species within the mesoporous silica (mSiO 2 ) channels to serve as a support for Ni-based CO 2 methanation catalysts. The results demonstrate that LaO x introduction (3.9 wt%) significantly improves CO 2 conversion from 38.2 % to 74.4 %, while enhancing CH 4 selectivity from 94.8 % to 99.7 % at 300 °C. Interestingly, excessive La loading does not noticeably reduce the promotion efficiency. Detailed characterization revealed that ultrafine LaO x species anchored within silica framework improved the dispersion and reduction of Ni nanoparticles and served as strong basic sites to promote CO 2 dissociation. In-situ DRIFT and isotope studies demonstrated that LaO x facilitated the hydrogenation of formate intermediates, enhancing both CO 2 conversion and CH 4 selectivity. In addition, LaO x endowed the support with hydrogen spillover capability, enabling active H from Ni nanoparticles to migrate to LaO x sites and accelerate the conversion of formate intermediates into CH 4 . These results underscore the potential of LaO x -modified mesoporous silica to optimize Ni-based catalysts, offering valuable guidance for the design of high-performance CO 2 hydrogenation catalyst supports.
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APPLIED ENERGY
·
2024
·
IF 10.1
Bingling Yuan,Zhen Chen,Qianxuan Zhang,Guoxiong Zhan,Lei Xing,Zhoulan Huang,Yuchen Li,Lidong Wang,Junhua Li
Chemisorption with biphasic solvents is a promising low-energy strategy for separating CO 2 from industrial flue gas, however, amine degradation and changes in water content can considerably impede the phase-splitting performance. To the issues, tetramethylene sulfone (TMS) was selected as separating agent to prepare a biphasic solvent with polyamine triethylenetetramine (TETA) with a TETA:TMS:H 2 O ratio of 2:6:2 (denoted as 20 T-60TMS). The CO 2 loading of the blended phase and the volume fraction of the rich phase were 2.56 mol/L and 35.4%, respectively; the total regeneration heat duty was 2.36 GJ/tCO 2 . The proposed biphasic solvent exhibited better resistance to oxidative degradation and thermal degradation than did previously reported solvents, attributed to the beneficial effect of TMS. Additionally, the degradation products did not substantially reduce the phase separation performance after a 360 h thermal degradation test. A dynamic phase-splitting evaluation revealed that the 20 T-60TMS solvent was robust to changes in water content. Theoretical calculations confirmed that the introduction of TMS weakened the hydrogen bond between TETACOO − /TETAH + and H 2 O, engendering enhanced TETACOO − and TETAH + self-aggregation, forming a strong hydrogen bond network, and achieving fast phase separation. This work provides a novel biphasic solvent with excellent tolerance and stability for CO 2 capture from flue gas.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Zhu Jiawei,Zhang Yu,Chen Zitao,Zhang Zhenbao,Tian Xuezeng,Huang Minghua,Bai Xuedong,Wang Xue,Zhu Yongfa,Jiang Heqing
Cu-oxide-based catalysts are promising for CO 2 electroreduction (CO 2 RR) to CH 4 , but suffer from inevitable reduction (to metallic Cu) and uncontrollable structural collapse. Here we report Cu-based rock-salt-ordered double perovskite oxides with superexchange-stabilized long-distance Cu sites for efficient and stable CO 2 -to-CH 4 conversion. For the proof-of-concept catalyst of Sr 2 CuWO 6 , its corner-linked CuO 6 and WO 6 octahedral motifs alternate in all three crystallographic dimensions, creating sufficiently long Cu-Cu distances (at least 5.4 Å) and introducing marked superexchange interaction mainly manifested by O-anion-mediated electron transfer (from Cu to W sites). In CO 2 RR, the Sr 2 CuWO 6 exhibits significant improvements (up to 14.1 folds) in activity and selectivity for CH 4 , together with well boosted stability, relative to a physical-mixture counterpart of CuO/WO 3 . Moreover, the Sr 2 CuWO 6 is the most effective Cu-based-perovskite catalyst for CO 2 methanation, achieving a remarkable selectivity of 73.1% at 400 mA cm −2 for CH 4 . Our experiments and theoretical calculations highlight the long Cu-Cu distances promoting *CO hydrogenation and the superexchange interaction stabilizing Cu sites as responsible for the superb performance.
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