COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yulan Xu,Minxian Wu,Xinlei Cheng,Shiying Wang,Dan Wang,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Gallium-based liquid metals are considered as promising catalysts for electrochemical CO 2 reduction due to their ability to effectively prevent the adhesion of byproduct carbon, which leads to the deactivation of electrode materials. In order to increase the specific area of liquid alloys, Ga-Sn thin liquid films were electrodeposited from a deep eutectic solvent composed of acetamide and dimethyl sulfone. Electrodeposition of Ga-Sn thin films with varying compositions that follow normal deposition behavior achieved, resulting in Sn rich in overall composition. To obtain Ga-rich thin liquid films, a straight forward and efficient two-step electrodeposition approach was employed. A layer of Ga thin film was firstly electrodeposited on the substrate, followed by electrodepositing a Sn layer. The prepared Ga-Sn thin films were applied for electrochemical reduction of CO 2 in a CO 2 -saturated 0.1 M KHCO 3 solution. Ga-Sn alloy with 91.6 at% Ga was in the liquid state at 25℃ and showed an excellent performance in reduction CO 2 to formate. The Faradaic efficiency reached 80 % and the partial current density was 46 mA cm −2 .
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MOLECULES
·
2024
·Vol. 29
·期 21
·4994
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IF 4.2
Fan Ma,Hong-Wei Lin,Zizi Li,Wen-Jing Li,Jia-Wei Wang,Gangfeng Ouyang
Noble-metal-free CO2reduction systems based on cobalt phthalocyanine (CoPc) and its derivatives have demonstrated remarkable photocatalytic performances; however, their structure-activity relationship with electronic tuning remains unexplored. Herein, we now provide a systematic study to investigate the electron effects of substituents on theCoPcfamily in photocatalytic CO2reduction, where a Cu(I) heteroleptic photosensitizer is utilized. The highest performance can be achieved using cobalt tetracarboxylphthalocyanine in light-driven CO2-to-CO reduction, with a maximum turnover number of 2950 at 450 nm and an outstanding apparent quantum yield of 63.5% at 425 nm, over ten times the activity with the tetra-dimethylamino-substitutedCoPcderivative. The favorable electron-withdrawing effects have been further verified by DFT calculations and cyclic voltammetry, which reduces the overpotential required for CO2reduction and decreases the Gibbs free energy of the catalyst active intermediates, particularly the CO-desorption energetics.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Minglun Cheng,Sibo Shen,Zhiwei Zhang,Kui Niu,Ning Wang
Electroreduction of CO2 to value-added low-carbon chemicals is a promising way for carbon neutrality and CO2 utilization. It was found that the diiron complex [(μ-bdt)Fe2(CO)6] (bdt = benzene-1,2-dithiolate) has high catalytic activity for electrocatalytic CO2 reduction. To further study the effect of the S-to-S bridge on the catalytic performances of diiron complexes for electrochemical CO2 reduction, four diiron complexes 1–4 with different rigid and conjugated S-to-S bridges were either selected or designed. The electrocatalytic studies showed that under optimal conditions, 2 with a 2,3-naphthalenedithiolato bridge exhibited the lowest catalytic onset potential (Eonset = −1.75 V vs Fc+/0), while 4 with a diphenyl-1,2-vinylidene bridge displayed the highest catalytic activity (TOFmax = 295 s–1), which is 1.5 times that of [(μ-bdt)Fe2(CO)6]. The controlled potential electrolysis experiments of 4 in 0.1 M MeOH/MeCN at −2.35 V vs Fc+/0 gave a total faradaic yield close to 100%, with selectivities of 77%, 9%, and 14% for HCOOH, CO, and H2, respectively. The mechanism for CO2 reduction was studied using density functional theory, IR spectroelectrochemistry, and electrochemical methods. The results indicate that modifying the structure of the S-to-S bridge is an effective strategy to improve the catalytic performance of diiron complexes for electrocatalytic CO2 reduction.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Yan Ouyang,Qi Liu,Tong Luo,Qinlan Luo,Min Xiao,Hongxia Gao,Zhiwu Liang
CO 2 loaded amine polymerizes during solvent regeneration at temperatures above 100 °C, resulting in the deterioration of solvent performance. Herein, five primary amines were heated to 120, 135 and 150 °C with CO 2 loading of 0.4C/N to study thermal degradation. It was found that 2-amine-1-butanol showed the greatest amine loss of 38.5 % after heating to 135 °C for 672 hrs while 2-amino-2-methyl-1-propanol was most stable with amine loss of 17.4 % under the same conditions. The degradation products were identified and the reaction pathway was studied through density functional theory (DFT) calculation. Furthermore, the transition state for ring closure and opening reactions was analyzed. The ring closure reaction to form oxazolidinones had a higher energy barrier, showing that it was the limiting step. This is further supported by the good agreement with experimental results. The structure–activity relationship showed the strong steric hindrance effect and the methyl group at β-carbon improved the amine stability.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fan Xu,Xin Meng,Rui Zhao,Daoming Jin,Wenhua Dai,Dandan Yang,Zhong Xin
The utilization of CO 2 for the production of light olefins through catalysis with iron-based catalysts presents a viable strategy to address the challenges of carbon neutrality. In this study, we synthesized a novel hybrid catalyst Fe 2 O 3 @ZrO 2 , derived from the pyrolysis of dual metal–organic frameworks (NH 2 -MIL-88B@UiO-66). Under specific conditions (340 °C, 3.0 MPa, CO 2 /H 2 = 1:3, 10000 mL g cat −1 h −1 ), the Fe 2 O 3 @ZrO 2 catalyst exhibited a notable space–time yield of light olefins at 12.7 mmol g −1 h −1 . The characterizations results show an electron transfer from ZrO 2 to the Fe 2 O 3 surface was observed at the heterointerface of Fe 2 O 3 and ZrO 2 . This electron transfer mechanism was identified as advantageous for the formation of the active phase Fe 5 C 2 . This research introduces an innovative use of the hybrid Fe 2 O 3 @ZrO 2 catalyst derived from MOF-on-MOF, holding significant promise in advancing the field of CO 2 hydrogenation catalysts.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xingbo Wang,Yibo Pan,Weidong Fan,Hao Guo,Hai Zhang
Municipal solid waste incineration (MSWI), a promising technology for managing MSWI capacity, has a large amount of CO 2 in its flue gas emissions, but lacks effective means of carbon reduction. Modification of CaO-based sorbents using fly ash, a solid waste from coal-fired power plants, is a potential application to improve CO 2 capture capacity. In this study, a cost-effective fly ash-CaO sorbent was developed by combining high-calcium and high-magnesium fly ash with CaO by hydration. The CO 2 capture capacity and carbonation conversion of fly ash-CaO sorbents were investigated at different temperatures, CO 2 partial pressures and doping ratios in a calcination/carbonation reaction system. Optimum carbonation reaction temperature (760℃) for CaO and optimum calcination temperature (850℃) for fly ash were obtained. In the experiment of CaO doped with fly ash, the novel sorbents prepared by CaO doped with fly ash at a mass ratio of 3:1 had the highest carbonation conversion (98.88 %). The hydration reaction promoted the transformation of CaO to Ca(OH) 2 , which improved the CO 2 capture capacity of the sorbents. The inert materials (Al 2 O 3 , SiO 2 ) in the fly ash were uniformly distributed as structural skeleton in the sorbents, enhancing the structural stability and anti-sintering ability. The S element contained in the fly ash competes with CO 2 for adsorption sites and produces stable CaSO 4 , which reduces the carbon capture capacity of the sorbents. A unique mineralization sequestration process for MSWI carbon capture is proposed that is economical and industrially viable. A promising route to improve CO 2 capture performance with waste reutilization is emphasized.
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Materials
·
2025
·Vol. 18
·期 7
·1443
·
IF 3.2
Yanshuang Chen,Yilin Chen,Hanqi Xu,Wenqi Zhao,Guodong Feng,Chunhui Xiao
The accumulation of coal gangue (CG), a byproduct of coal mining, poses severe environmental challenges. This study presents a green strategy to convert CG into high-value NaX zeolite via an alkali fusion–hydrothermal method. Through orthogonal experiments, the optimal synthesis conditions (solid–liquid ratio 1:8, crystallization temperature 110 °C, time 12 h) were identified, yielding NaX zeolite with exceptional crystallinity (98%), specific surface area (703.5 m2/g), and pore volume (0.28 cm3/g). Comprehensive characterization (XRD, SEM-EDS, BET, etc.) confirmed its structural integrity and thermal stability. The synthesized zeolite exhibited remarkable adsorption capacities for Cu2+(185.35 mg/g) and CO2(5.51 mmol/g), following the Langmuir isotherm model. This work not only addresses gangue disposal challenges but also demonstrates a cost-effective route for producing high-performance adsorbents, aligning with circular economy and carbon neutrality goals.
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CRYSTENGCOMM
·
2025
·
IF 2.6
Ming-Li Ma,Le-Chen Zheng,Rui Li,Yabo Xie
MOF@COF heterostructures featuring abundant porosity, designable structures and efficient separation of photogenerated charge carriers are enthusiastically embraced as promising candidates for the capture and conversion of CO2. Nonetheless, the laborious synthesis procedures involving energy-consuming protection and degassing steps severely impede their widespread application. In this study, a concentration-acid co-regulation strategy was developed to synthesize highly efficient MOF@COF composites in atmospheric air, obviating the need for vacuum, inert gases, and/or repeated freezing. With reduced supersaturation of the synthesis mixtures and intensified competitive coordination from acid modulators, the crystallization of COFs was strategically confined to the exterior surfaces of MOFs, fostering intimate contact to facilitate the interphase electron transfer. The synthesized MOF@COF heterostructures thereby exhibited radically enhanced CO2RR performances, yielding ca. 2.5 times more CO than the original deficiently-contacted composite. Moreover, the versatility of the synthesis strategy was validated using altered MOF and COF structures, shedding light on the significance of crystallization regulation in fabricating advantageous heterostructures. These findings are poised to effectively propel the development and practical implementation of MOF@COF composites.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yao Shen,Ke Wang,Lu Li,Jingkai Zhao,Jiexu Ye,Ping Chen,Xiang Gao,Shihan Zhang
Catalyst-aided CO 2 desorption offers a promising reduction in the energy penalty of amine scrubbing, but faces the challenges of slow mass transfer, sluggish desorption kinetics, and susceptibility to deactivation. In this work, a hollow composite catalyst C@ZrO 2 was developed to simultaneously realize rapid electron, proton and mass transfer for CO 2 desorption via facilitating proton-coupled electron transfer (PCET) effect. The CO 2 desorption rate of benchmark MEA solution increased by 126% and relative heat duty decreased by 69.9% in presence of C@ZrO 2 , and its catalytic performance didn’t noticeably decline after 10 cycles. Additionally, the desorption rate of biphasic solvents with a high viscosity increased by 112% and relative heat duty decreased by 57.3% with C@ZrO 2 . Based on theoretical calculation, the facilitated PCET efficiency of carbon layer increased the binding energy of carbamate to enhance its mass transfer rate from the liquid phase to the C@ZrO 2 surface, and stretched the C-N bond to reduce the proton transfer energy barrier by 66.8%. This work provided a novel insight to design catalysts for energy-efficient and stable CO 2 capture.
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RARE METALS
·
2024
·
IF 9.6
Wan Si-Jie,Hou Yan-Ting,Wang Wang,Luo Guo-Qiang,Wang Chuan-Bin,Tu Rong,Cao Shao-Wen
Photocatalytic reduction of CO 2 has attracted considerable interest owing to its potential to resolve the energy and environmental problems. Nevertheless, the lack of proficient photocatalysts has restricted the application of solar-driven photocatalytic CO 2 reduction. Herein, we reported an S-scheme heterojunction by combining g-C 3 N 4 with La 3+ and Rh 3+ co-doped SrTiO 3 through the electrostatic self-assembly method for the efficient photocatalytic CO 2 reduction. In comparison with g-C 3 N 4 , the as-prepared CN/LRSTO-30 wt% S-scheme heterojunction not only possesses a broadened visible-light response due to the defect states in La, Rh co-doped SrTiO 3 induced by co-doped La 3+ and Rh 3+ but also has more adsorption sites for the capture and activation of CO 2 molecules. Additionally, separation and transfer efficiency of the photoinduced charge carriers is much enhanced in the CN/LRSTO-30 wt% S-scheme heterojunction via its robust internal electric field, which is firmly demonstrated by in situ irradiation X-ray photoelectron spectroscopy technology. Consequently, the prepared S-scheme heterojunction achieves impressive photocatalytic CO 2 reduction performance with an average CO and CH 4 evolution rate of 4.1–1.8 μmol·g −1 ·h −1 , respectively, which are ~ 1.9 and ~ 22.5-fold higher than those of pure g-C 3 N 4 . This study provides innovative perspectives on the design of creative S-scheme heterojunctions for applications in photocatalytic CO 2 reduction. Graphical abstract
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Journal of the American Chemical Society
·
2024
·
IF 14.4
Fan Ma,Zhi-Mei Luo,Jia-Wei Wang,Gangfeng Ouyang
The development of efficient, selective, and durable CO2 photoreduction systems presents a long-standing challenge in full aqueous solutions owing to the presence of scarce CO2 and the fierce competition against H2 evolution, which is even more challenging when noble metals are not utilized. Herein, we present the facile decorations of four phosphonic acid groups on a donor–acceptor-type organic dye to obtain a water-soluble photosensitizer (4P-DPAIPN), which succeeds the excellent photophysical and photoredox properties of its prototype, exhibiting long-lived delayed fluorescence (>10 μs) in aqueous solutions. Combining 4P-DPAIPN with a cationic cobalt porphyrin catalyst has accomplished record-high apparent quantum yields of 9.4–17.4% at 450 nm for CO2-to-CO photoconversion among the precedented systems (maximum 13%) in fully aqueous solutions. Remarkable selectivity of 82–93% and turnover number of 2700 for CO production can also be achieved with this noble-metal-free system, outperforming a benchmarking ruthenium photosensitizer and a commercial organic dye under parallel conditions. Such high performances of 4P-DPAIPN can be well maintained under real sunlight. More impressively, no significant decomposition of 4P-DPAIPN was detected during the long-term photocatalysis. Eventually, the photoinduced electron transfer pathways were proposed.
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Journal of Physical Chemistry C
·
2024
·
IF 3.3
Tongxin Xiao,Xige Wu,Hongbao Liang,Kangyue Qiao,Ying Chen
Solar-powered photocatalytic conversion of CO2 into green solar fuels is one of the effective ways to solve the global energy crisis and the greenhouse effect. A new artificial photosynthesis system composed of TiO2 nanotube arrays (TiO2NTs) and bimetallic porphyrin was fabricated, and their photocatalytic activities were evaluated by the reduction of gas-phase CO2 to CH4 under simulated solar irradiation. Compared to pure TiO2NTs and CoTCPP/TiO2NTs, bimetallic porphyrin-sensitized TiO2NTs displayed greatly ameliorated photocatalytic activity. Among them, Ni-CoTCPP/TiO2NTs exhibited the highest photoreduction efficiency, and the reduction rate of CO2 into CH4 was up to 52.27 μmol/cm2/h with the quantum efficiency of 1.002%, about 7 times higher than that of pure TiO2NTs. The increase in photocatalytic performance can be attributed to the enhancement of the light absorption capacity of Ni-CoTCPP/TiO2NTs and the higher charge separation efficiency. Furthermore, according to the results of the photocatalytic evaluation and photo(electro)chemical studies, a possible mechanism of CO2 photoreduction over Ni-CoTCPP/TiO2NTs was proposed.
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