JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
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IF 6.1
Wei Rong,Meili Ding,Pan Ma,Suyu Kong,Jianfeng Yao
Accumulation of atmospheric CO 2 poses a serious threat to the global environment, but there is still a lack of effective CO 2 catalytic conversion under mild conditions. Herein, multifunctional ZnO/N-doped porous carbon materials, ZNPC-X, were fabricated by pyrolysis of available pine pollen with melamine and zinc chloride . The optimized ZNPC-600 produced at 600 °C can work as an efficient photothermal catalyst towards CO 2 cycloaddition conversion with a high catalytic yield of 99% under mild conditions (0.3 W/cm 2 , 1 bar). Moreover, ZNPC-600 shows excellent recyclability after ten cycles and desirable performance even under simulated flue gas and after moisture treatment. Absorption spectra and time-dependent infrared images unveil that the intrinsically broad light absorption and high photothermal conversion efficiency are the major reasons for the high activity of ZNPC-600. Besides, photogenerated electrons can be transferred to CO 2 and activate it, while photogenerated holes can be used as Lewis acid to facilitate the ring opening of epoxides. In addition, the hierarchical pore structure and the synergy between ZnO and pyridine N also play a role in the mass transfer and activation of epoxides and CO 2 , respectively. This work provides a low-cost and facile solution to obtain catalysts derived from biomass for promoting CO 2 conversion.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Chen Wang,Yan Zhu,Yihan Ling,Yansheng Gong,Rui Wang,Huanwen Wang,Jun Jin,Ling Zhao,Beibei He
Solid oxide electrolysis cells (SOECs) show great promise in converting CO2 to valuable products. However, their practicality for the CO2 reduction reaction (CO2RR) is restricted by sluggish kinetics and limited durability. Herein, we propose a novel medium-entropy perovskite, Sr2(Fe1.0Ti0.25Cr0.25Mn0.25Mo0.25)O6−δ (SFTCMM), as a potential electrode material for symmetrical SOEC toward CO2RR. Experimental and theoretical results unveil that the configuration entropy of SFTCMM perovskites contributes to the strengthened metal 3d–O 2p hybridization and the reduced O 2p bond center. This variation of electronic structure benefits oxygen vacancy creation and diffusion as well as CO2 adsorption and activation and ultimately accelerates CO2RR and oxygen electrocatalysis kinetics. Notably, the SFTCMM-based symmetrical SOEC delivers an excellent current density of 1.50 A cm–2 at 800 °C and 1.5 V, surpassing the prototype Sr2Fe1.5Mo0.5O6−δ (SFM, 1.04 A cm–2) and most of the state-of-the-art electrodes for symmetrical SOECs. Moreover, the SFTCMM-based symmetrical SOEC demonstrates stable CO2RR operation for 160 h.
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Advanced Energy Materials
·
2023
·Vol. 13
·期 42
·2302692
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IF 27.8
Qingyu Wang,Yida Zhang,Minxi Lin,Hengwei Wang,Yu Bai,Chengyuan Liu,Junling Lu,Qiquan Luo,Gongming Wang,Hai-Long Jiang,Tao Yao,Xusheng Zheng
Metastable structures are promising candidates for efficient catalysis owing to abundant active electronic states, strong electronic coupling with reactants, and energetic preference. Exerting the value of metastable structures while evading the difficulty in direct synthesis remains challenging. Herein, it is reported that light irradiation enables the generation and maintenance of the metastable state over copper single atoms for efficient carbon dioxide reduction. Under irradiation with light, photogenerated electrons transit to Cu-3 d orbits and initiate d -orbital rearrangement. The initial symmetric Cu 1 ─O 4 coordination converts to the metastable asymmetric structure of Cu 1 ─O 2+1 , and is reversibly restored after removing the light. The photoinduced metastable intermediate of Cu 1 ─O 2+1 promotes the Cu single-atom catalyst to deliver an ethylene yield rate of 60.4 µmol g cat. −1 h −1 . Mechanistic studies reveal that Cu 1 ─O 2+1 possesses stronger adsorption capability for reactants and intermediates. The reaction energy barrier over Cu 1 ─O 2+1 also shows an obvious decline compared to that over Cu 1 ─O 4 .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shuhui Xia,Chaolong Wei,Yong Zhai,Bin Ding,Jianyong Yu,Jianhua Yan
Photocatalytic CO 2 reduction is an attractive strategy to realize carbon–neutral economy but is challenging by its low efficiency and uncontrollable selectivity. Here, we report a new flexible black BaTiO 3 nanofiber (B-BTO NF) and prove its unique function of ultrasonic cavitation enhanced photocatalytic CO 2 reduction into controllable syngas. The B-BTO NFs with a large deformation ability and a high mechanical strength contain unsaturated Ti 3+ coordination and vacancy defects. Under ultrasound, the NF film gathers abundant cavitation bubbles, and the continual explosions of these bubbles bring periodic piezoelectric polarization changes and release net charges on B-BTO NFs, thus triggering photocatalytic CO 2 reduction into syngas. Moreover, the product selectivity can be controlled by facilely adjusting the ultrasonic frequency and power. As a result, the evolution rate of target syngas (CO/H 2 ≈ 1:1.3) reaches as high as 12525 μmol/g/h. The proposed flexible B-BTO NF induced ultrasonic cavitation-enhancement strategy provides new insights for designing photocatalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Zhiwei Jian,Jiangwei Yu,Ian Jimmy Madatta,Yang Liu,Jinrui Ding
The electrochemical reduction of carbon dioxide (CO 2 ) to high-energy multi-carbon compounds is a significant challenge. Efforts have been made to design efficient catalysts for high selectivity toward multi-carbon products. In this study, granular protruded irregular Cuprous oxide (Cu 2 O) nanoparticles were synthesized using a simple water bath wet chemical reduction method. Polyethylene glycol (PEG) was utilized as a directing agent to control the morphology of Cu 2 O in the process. The optimized irregular Cu 2 O (ir-Cu 2 O) catalyst exhibits a remarkable faraday efficiency of 69.3% (±3.3%) for double-carbon compounds (C 2 ), which is significantly higher than that of polyhedral Cu 2 O (p-Cu 2 O) (50.4%±1.1%) synthesized without adding PEG . Cu 2 O nanoparticles with irregular shape featuring randomly distributed spherical protrusions offer more active sites for CO 2 adsorption than p-Cu 2 O catalysts, which is beneficial for the conversion of CO 2 to C 2 . In addition, in situ infrared spectra reveal that ir-Cu 2 O reduces CO 2 to C 2 mainly through the coupling of the CO* and CHO*, thereby promoting the formation of C 2 . These findings provide valuable insights for the design of high-efficiency electrocatalysts for CO 2 electroreduction to C 2 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
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IF 9.446
Xiahui Lin,Yilin Gao,Min Jiang,Yongfan Zhang,Yidong Hou,Wenxin Dai,Sibo Wang,Zhengxin Ding
Herein, we report the facile synthesis of uniform perovskite hydroxide CoSn(OH) 6 nanocubes and their first use as noble-metal-free, highly efficient and stable catalysts for the deoxygenative reduction of CO 2 to CO with visible light. The CoSn(OH) 6 sample is synthesized through a one-pot co-precipitation method and fully characterized by various techniques including XRD, FTIR, FESEM, TEM, EDX, EDX-mappings, XPS, DRS, and N 2 sorption measurements. The CoSn(OH) 6 solid is found by theoretical calculations to be capable of absorbing and activating CO 2 molecules on the (100) surface. Under the optimal reaction conditions, the CoSn(OH) 6 catalyst exhibits a high CO 2 reduction activity with visible light irradiation, affording a CO generation rate of 18.7 μmol h −1 . The stability and reusability of the CoSn(OH) 6 catalyst for photocatalytic CO 2 reduction are solidly confirmed. Results of in situ photoluminescence spectroscopy and photocurrent response characterizations indicate that the CoSn(OH) 6 catalyst can efficiently promote the separation and transfers of photoexcited charge carriers during photocatalysis, and eventually leading to obviously enhanced CO 2 photoreduction performance. Moreover, a possible mechanism for the photocatalytic CO 2 reduction reaction is also proposed based on the results of activity evaluation and photo-/electro-chemical measurements.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhixiu Yang,Xiu Wen,Xiaoxuan Guo,Yong Chen,Ruiping Wei,Lijing Gao,Xiaomei Pan,Jin Zhang,Guomin Xiao
The electrochemical CO 2 reduction to specific multi-carbon product on copper-based catalysts is subjected to low activity and poor selectivity . Herein, catalyst structure, morphology, and chemical component are systematically studied for bolstering the activity and selectivity of as-prepared catalyzers in this study. Dendritic fibrous nano-silica spheres favor the loading of active species and the transport of reactant from the central radial channel. Cu/DFNS with high dispersion active sites are fabricated through urea-assisted precipitation way. The coexistence of Cu(I)/Cu(II) induces a close combination of Cu active sites and CO 2 on the Cu/DFNS interface, promoting the CO 2 activation and C C coupling. The Cu–O–Si interface (Cu phyllosilicate) can improve CO 2 and CO attachment. Cu/DFNS show the utmost Faradaic efficiency of C 2 H 4 with a value of 53.04% at −1.2 V vs. RHE. And more importantly, in-situ ATR-SEIRAS reveals that the C C coupling is boosted for effectively producing C 2 H 4 as a consequence of the existence of *CO L , *COOH, and *COH intermediates. The mechanism reaction path of Cu/DFNS is inferred to be *CO 2 → *COOH → *CO → *CO*COH → C 2 H 4 . Our findings will be helpful to gain insight into the links between morphology, texture, chemical component of catalyzers, and electrochemical reduction of CO 2 , providing valuable guidance in the design of more efficient catalysts.
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INORGANIC CHEMISTRY
·
2023
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IF 4.6
Hua-Qing Yin,Ming-Yang Cui,Hao Wang,Yuan-Zhao Peng,Jia Chen,Tong-Bu Lu,Zhi-Ming Zhang
Carbon dioxide cycloaddition into fine chemicals is prospective technology to solve energy crisis and environmental issues. However, high temperature and pressure are usually required in the conventional cycloaddition reactions of CO2 with epoxides. Moreover, metal active sites play a vital role in the CO2 cycloaddition, but it is still unclear. Herein, we select the isostructural MOF-919-Cu-Fe and MOF-919-Cu-Al as models to promote the performance and clarify the effects of metal type on the CO2 cycloaddition. The MOF-919-Cu-Fe with exposed Fe and Cu Lewis acid sites reaches the CO2 cycloaddition with over 99.9% conversion and over 99.9% selectivity at room temperature and a 1 bar CO2 atmosphere, 3.0- and 52.6-fold higher than those of the MOF-919-Cu-Al with Al and Cu sites (33.8%) and the 1H-pyrazole-4-carboxylic acid, Fe, and Cu mixed system (1.9%), respectively. The proposed mechanism demonstrated that the exposed Fe3+ sites facilitate the ring opening of epoxide and CO2 activation to boost the CO2 cycloaddition reaction. This work provides a new insight to tune the catalytic sites of MOFs to achieve high performance for CO2 fixation.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Junjian Yu,Zhe Wang,Cancan Yang,Fei Wang,Yanyin Cheng,Song Wang,Yi Zhang,Zhaoli Wang
Metal-organic frameworks (MOFs) are one of the optimal choice to be endowed for designing high-performance CO 2 separation membranes as the fillers, ascribing their unprecedented tunability and chemical functionalities. However, while pursuing more types of MOFs, researchers have slightly explored their inherent properties. Thus, we incorporated missing-linker defects into Zirconium Metal−Organic Framework for tailoring the superior CO 2 transport channel through tune their microporosity . And a series of defect-engineered UiO-66 (UiO-AcOH) fillers were synthesized and mingled into PIM-based matrix with large free volume. Resistance model simulations and gas permeation tests confirmed that the defective UiO-66 can greatly improved the competitive adsorption of the dispersed phase in Mixed Matrix Membranes (MMMs), offering more degree of freedom for the transportation of CO 2 . At the optimal ratio, the CO 2 permeability of the UiO-AcOH-1.4/PIM-15 wt% MMMs increased nearly 3.5 times (CO 2 =11261 Barrer, and the CO 2 /N 2 selectivity is 26, almost increasing 23% contrasted pure film. Moreover, MMMs possess excellent long-term working stability and anti-aging properties, showing excellent gas separation performance.
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ENERGY & FUELS
·
2023
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IF 5.3
Chen Huang,Ying Zhang,Shuofan Li,Quan Shi,Suoqi Zhao,Linzhou Zhang
With the escalating global energy crisis and burgeoning environmental concerns as a result of the accumulation of used lubricating oil, the urgency and economic potential of recycling this waste is undeniably critical. Conventional methods, such as distillation and hydrogenation, often stumble upon operational difficulties as a result of thermochemical decomposition, while advanced procedures, like molecular distillation and membrane separation, face industrial scale-up, owing to prohibitive costs and limited separation capabilities. Herein, this study heralds the emergence of supercritical CO2 (SC-CO2) extraction, which can exemplify superior efficacy in addressing these concerns. Leveraging the high solvency under extreme pressure and low-temperature conditions, SC-CO2 can selectively separate undesirable components, reducing coke formation and simplifying subsequent refining stages. The comprehensive analysis, conducted using gas chromatography–mass spectrometry and high-resolution mass spectrometry, revealed the selectivity of SC-CO2 toward saturates with a smaller molecular weight. On the basis of this analysis, the optimal extraction condition was determined. Implementing a two-stage process at 70 °C and 10–20 MPa, we effectively eradicated residual small molecules and large polar compounds, yielding an intermediate fraction rich in isoparaffins and 1–4 ring naphthenes with a carbon distribution of C25–40. Notably, the recovery rate of saturates was 60%. Critically, the removal rate of undesirable components in recycled lubricating oil is remarkably high, reinforcing the practical viability and exceptional advantages of SC-CO2 extraction for lubricating oil recycling as a sustainable and economically rewarding solution to pressing global energy and environmental predicaments.
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ChemCatChem
·
2023
·Vol. 15
·期 18
·e202300605
·
IF 4.5
Boyu Zhu,Jinling Hu,Youting Wu,Jiao Geng,Xingbang Hu
Graphical This paper presented a pioneering attempt to employ knitting aromatic polymers (KAPs) immobilized with RuCl 3 as catalysts for formate synthesis. TON as high as 1470000 with an average TOF of 122500 h −1 can be achieved, which are obviously higher than other reported heterogeneous Ru or Ir catalysts. The catalyst can be easily recovered and reused. There is widespread interest in the hydrogenation of CO 2 to produce high-energy substances such as formic acid. Herein, ruthenium trichloride was immobilized on porous phosphine polymers (Ru/KAPs-Ph-PPh 3 ) and gave excellent catalytic activity in the hydrogenation of CO 2 to produce formate. With the assistance of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU), a high turnover number (TON) of up to 1470000 was obtained in 12 hours at 120 °C and a total pressure of 6 MPa (P(H 2 )/P(CO 2 )=1 : 1), with average TOFs of 122500 h −1 . Moreover, the catalyst can be easily recovered by filtration with acceptable catalytic effectiveness.
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Materials Today Sustainability
·
2023
·
IF 7.8
X. Wang,P. Ma,Y.J. Jing,C. Yu,H. Qiu,C. Kang,Z. Cui,K. Hou,A.C.K. Yip,B.H. Yin
Excessive emission of greenhouse gases has caused global warming and been seriously damaging the ecological environment. Adsorption technology is one of the most powerful methods widely used for carbon capture. However, the currently available rigid porous adsorbents are all insoluble, the regeneration of which once blocked is a quandary. In this study, we synthesized a soluble polymeric adsorbent of intrinsic microporosity (AO-PIM-1) for carbon dioxide (CO 2 ) capture. The adsorbent of AO-PIM-1, an amidoxime functionalized PIM-1, possesses a high-specific surface area of 503 m 2 /g and a strong affinity for CO 2 with the heat of adsorption of 30.6 kJ/mol. It exhibits high CO 2 adsorption capacity and CO 2 /N 2 selectivity evidenced by computational calculations and experimental breakthrough experiments. More importantly, the microporous AO-PIM-1 is well soluble in common organic solvents like DMF, DMSO, and DMAc, but insoluble in methanol, which allows the regeneration, once being fouled, with a solvent dissolution-separation purification-nonsolvent-induced precipitation (DSP) method.
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