ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Xiaoyang Chen,Jian Chen,Yijie Liu,Yang Liu,Yun Gao,Siwei Fan,Xiangxi He,Xiaohao Liu,Chao Shen,Yong Jiang,Li Li,Yun Qiao,Shulei Chou
Metal–CO2 batteries, especially Li–CO2 and Na–CO2 batteries, are regarded as ideal new-generation energy storage systems owing to their high energy density and extraordinary CO2 capture capability. However, the advancement of metal–CO2 batteries is still at an early stage. The problems caused by accumulation of carbonates during charge–discharge cycles, such as large polarization and poor reversibility, restrict their practical application. Therefore, designing efficient catalysts is crucial for promoting the decomposition of carbonate to improve the electrochemical performance of metal–CO2 batteries. Herein, we first adopted sea urchin-like γ-MnO2 as the cathode material for Li/Na–CO2 batteries. Benefiting from the unique structure and excellent catalytic activity of γ-MnO2, the as-prepared Li–CO2 and Na–CO2 batteries can achieve low overpotentials of 1.28 and 1.36 V, respectively, at a current density of 100 mA g–1 with a cutoff capacity of 1000 mA h g–1. The overpotentials are lower than those of most of the state-of-the-art catalysts in previous reports. After 100 and 50 cycles of Li–CO2 and Na–CO2 batteries, respectively, their charging termination voltages remain at around 4.1 and 3.9 V, respectively; such a low charging platform indicates the excellent catalytic activity of the γ-MnO2 cathode on the discharge products. Our findings offer a promising guideline to design efficient electrocatalysts for high-performance metal–CO2 batteries.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Ting Liang,Jingwen Wei,Shiming Zhang,Jinhang Yang,Jiangli Sun,Zuji Li,Zhihong Li,Zebin Yu,Shuangfei Wang,Yanping Hou
Design of photocatalysts with high-efficiency for sunlight utilization is one of the prerequisites for CO 2 photoreduction . Besides, modulating a stable electron-donating environment to meet the energy barrier for CO 2 reduction to CO is crucial. In this work, the ZnSe/Ag 2 Se/AgBr (ZAA) heterojunction was fabricated by growing the ZnSe on the AgBr surface accompanied by in-situ generation of Ag 2 Se between the two components by hydrothermal process. Results showed that the ZAA exhibited excellent light response ability over the full wavelength range. X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) demonstrated that the charge transfer of the ZAA conformed to dual Z-scheme mechanism, with the Ag 2 Se acting as an electron transfer bridge, which in turn acted as an electron reservoir to accelerate electron transfer, facilitating carriers’ separation. The highest CO yield of 54.14 µmol/g/h was obtained from the optimal ZAA-2, which was 11.76 and 10.44 times of pure ZnSe and Ag 2 Se, respectively. This work demonstrated the feasibility of a dual Z-scheme heterostructure with full spectrum response for offering stable electron-donating environment and improving electron transfer for enhanced photocatalytic activity.
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CARBOHYDRATE POLYMERS
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2023
·
IF 11.2
Ziteng Liu,Peng Wei,Ying Qi,Xueli Huang,Yahong Xie
The injection of CO 2 into oil reservoirs to enhance oil recovery (EOR) has become a widely accepted and effective technical method, which, however, remains subject to the gas channeling caused by the reservoir fractures. Herein, this work developed a novel plugging gel combining excellent mechanical properties, fatigue resistance, elastic and self-healing properties for the CO 2 shutoff purpose. This gel consisting of grafted nanocellulose and polymer network was synthesized via a free-radical polymerization, and reinforced by using Fe 3+ to cross-link the two networks. The as-prepared PAA-TOCNF-Fe 3+ gel has a stress of 1.03 MPa and a high strain of 1491 %, and self-heals to its original 98 % in stress and 96 % in strain after rupture, respectively. The introduce of TOCNF/Fe 3+ improves the excellent energy dissipation and self-healing via the synergy effect of dynamical coordination bonds and hydrogen bonds . Further, the PAA-TOCNF-Fe 3+ gel is both flexible and high-strength in plugging the multi-round CO 2 injection, during which the CO 2 breakthrough pressure is above 9.9 MPa/m, the plugging efficiency exceeds 96 %, and the self-healing rate is larger than 90 %. Given that above, this gel shows a great potential to plug the high-pressure CO 2 flow, which could offer a new method for CO 2 -EOR and carbon storage.
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Processes
·
2023
·Vol. 11
·期 4
·1075
·
IF 3.5
Zhaochen Huang,Guoqiang Huang
Usually, the ion implantation gases used in semiconductor production are required to be extremely high in purity. Due to the presence of trace CO2in electronic special gas BF3, the quality of the material is significantly affected, which makes it crucial to impose control on CO2content. Unlike a series of blank adsorbents reported in other studies, the zinc-loaded adsorbents prepared in this study are intended for the adsorption of CO2from CO2/BF3. Firstly, the materials were characterized by XRD, BET, SEM-EDS and TG-DSC analysis, etc., and the breakthrough curves of the adsorbents as obtained under different preparation conditions were investigated at 20 °C and 200 kPa. The results show that the adsorption performance reached the optimal level when the activation temperature was 450 °C and a 13X molecular sieve was impregnated by 0.15 mol/L Zn(NO3)2. Moreover, compared with the Zn-13X, the breakthrough time was reduced to 69% and 44% in two adsorption cycles, respectively. Finally, FTIR was used to reveal the adsorption mechanism of the carbonates produced by CO2adsorption. It was found that the adsorption performance was affected by the irreversible reduction in the number of active sites due to the continuous formation of polydentate carbonate during adsorption and regeneration.Keywords:CO2adsorption;13X molecular sieve;carbonate species
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Zhang Jin,Guo Chenxi,Fang Susu,Zhao Xiaotong,Li Le,Jiang Haoyang,Liu Zhaoyang,Fan Ziqi,Xu Weigao,Xiao Jianping,Zhong Miao
Electrochemical CO 2 reduction (CO 2 R) to ethylene and ethanol enables the long-term storage of renewable electricity in valuable multi-carbon (C 2+ ) chemicals. However, carbon–carbon (C–C) coupling, the rate-determining step in CO 2 R to C 2+ conversion, has low efficiency and poor stability, especially in acid conditions. Here we find that, through alloying strategies, neighbouring binary sites enable asymmetric CO binding energies to promote CO 2 -to-C 2+ electroreduction beyond the scaling-relation-determined activity limits on single-metal surfaces. We fabricate experimentally a series of Zn incorporated Cu catalysts that show increased asymmetric CO* binding and surface CO* coverage for fast C–C coupling and the consequent hydrogenation under electrochemical reduction conditions. Further optimization of the reaction environment at nanointerfaces suppresses hydrogen evolution and improves CO 2 utilization under acidic conditions. We achieve, as a result, a high 31 ± 2% single-pass CO 2 -to-C 2+ yield in a mild-acid pH 4 electrolyte with >80% single-pass CO 2 utilization efficiency. In a single CO 2 R flow cell electrolyzer, we realize a combined performance of 91 ± 2% C 2+ Faradaic efficiency with notable 73 ± 2% ethylene Faradaic efficiency, 31 ± 2% full-cell C 2+ energy efficiency, and 24 ± 1% single-pass CO 2 conversion at a commercially relevant current density of 150 mA cm −2 over 150 h.
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ChemistrySelect
·
2023
·Vol. 8
·期 13
·e202202681
·
IF 2.1
Qing-Qing Pang,Xi-Zheng Fan
Graphical The ultra-fine Pd nanoparticles (NPs) are constructed by strong electrostatic adsorption strategy to ensure ample active sites, further enhance the light absorption intensity and optimize the separation efficiency of electron and hole, contributing to dramatically promote the performance of photocatalytic CO 2 reduction and stability in the gas-solid phase system. The photocatalytic CO 2 converted into the value-added products is regarded as a green strategy for the conversion and utilization of energy. Herein, we develop a commodious SEA (strong electrostatic adsorption) strategy to synthesize Pd-based photocatalysts with ultra-fine Pd NPs (Pd/TiO 2 −S−B). As verified by experiments and characterizations, the ultra-fine Pd NPs can inexorably heighten the reaction activity of catalyst, because it can provide several functions consist of improving the carrier separation efficiency, light absorption and CO 2 molecules adsorption. Meanwhile, the interaction of Pd and substrate can prevent the agglomeration of Pd NPs in reaction process. The designed Pd/TiO 2 −S−B contributes excellent performance in a gas-solid system. The yields of CO (105.1 μmol/g-cat) and CH 4 (254.3 μmol/g-cat) detected, are about 5.25 and 6.24-fold higher than those of pristine TiO 2 . Pd/TiO 2 −S−B also exhibits the forceful stability with acceptable decline of catalytic activity after three cycles. This opens the door for the preparation of high-performance and steady photocatalysts by reliable and effortless strategies toward CO 2 reduction.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
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2023
·Vol. 224
·期 18
·2300036
·
IF 2.5
Wei Zhang,Yi Sun,Yiting Xu,Xiaobo Yu,Yajin Fang,Fei Liu,Haining Na,Jin Zhu
Fabrication of fluorescent cellulose with aggregation-induced emission (AIE) characteristics is usually achieved by grafting tetraphenylethylene (TPE) to the cellulose backbone using TPE derivatives with highly active functional groups such as carboxylic, isothiocyanate, and alkynyl groups. However, besides the complicated synthetic routes of these TPE derivatives, conversion of hydroxyl groups in the cellulose chain to more reactive groups such as amine or azide groups is usually involved, and the resulting products have a degree of substitution (DS) of TPE lower than 0.08. Herein, a facile one-pot strategy for the grafting of a TPE group to the cellulose backbone with high DS of up to 0.22 in a CO 2 switchable solvent under mild reaction conditions is reported. The hydroxyl groups in the cellulose are in situ converted to cellulose carbonate intermediately during the dissolution step. Subsequently, nucleophilic substitution between the intermediate and a halogenated TPE derivative with bromine atom as leaving group is carried out to achieve the effective grafting of TPE. The synthetic route for this promising TPE derivative is much more convenient than those of TPE derivatives reported in previous studies. This work suggests a new and facile pathway for the synthesis of high-emission fluorescent cellulose with AIE functionality.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Ning Sun,Mingwei Gao,Jiawei Liu,Guang Zhao,Fei Ding,Qing You,Caili Dai
With the increasing demand for oil and gas resources, deep tight oil and gas reservoirs have gradually become the focus of global oil and gas exploration and development. Hydraulic fracturing technology based on water-base fracturing fluid plays a more and more important role in improving the recovery of tight oil reservoirs. Under the background of global CO 2 emission reduction, a CO 2 -responsive clean fracturing fluid with controllable gelling/gel breaking at high temperatures was constructed in this paper. The system was not only friendly to the reservoir and environment, but also overcame the shortcomings of the traditional clean fracturing fluid with undesirable temperature resistance. The viscosity characteristics and viscoelastic behavior of temperature-resistant clean fracturing fluid were investigated through high-temperature rheology experiments. The interaction between fluid and rock was investigated through the core flow experiment. The results showed that the clean fracturing fluid had the characteristics of good CO 2 responsiveness, excellent shear resistance at high temperatures, high drag reduction, satisfactory gel breaking performance, low filtration and low core damage. The complex three-dimensional network structure formed by the intertwined micelles and vesicles improves the temperature resistance of the clean fracturing fluid. It is expected that the fluid can not only be used to improve oil recovery in tight oil reservoirs, but also be used to solve the leakage problem in CO 2 storage underground.
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ChemElectroChem
·
2023
·Vol. 10
·期 7
·e202201147
·
IF 4
Xinzuo Fang,Sheng Lei,Zhiwei Feng,Junfei Ou
Graphical Enhanced conductivity : Al−PMOF−Cu−PPy are obtained through metallization of the porphyrin linkers followed by polymerization of pyrrole, which exhibit enhanced photocatalytic activity for CO 2 reduction. DFT calculations reveals the electron interaction between the polypyrrole and the MOFs can narrow the band gap, promote the electron transition and thus enhance the photocatalytic activity. Photocatalytic CO 2 reduction to valuable fuels is highly desirable to alleviate global warming and energy crisis. Herein, a stable aluminum-porphyrin metal-organic frameworks (MOFs) named Al−PMOF, with wide spectral response, is selected as platforms for the construction of efficient photocatalyst to convert CO 2 into CO. To enhance the activity of pristine Al−PMOF, highly active reaction sites are introduced through metallization of the porphyrin linkers with Cu 2+ . Furthermore, the polymerization of pyrrole in the channel of MOFs is also performed to improve the electron conductivity and narrow the band gap. The polypyrrole offers the conductive network to transfer the light-generated electrons and thus enhances the efficient charge separation. The calculated electronic density of states based on the density functional theory (DFT) further prove the electron interaction between the polypyrrole and the MOFs, which benefit the enhancement of photocatalytic performance of Al−PMOF.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Yichao Tong,Changlei Qin,Xianqing Zhu,Zongze Lv,Xin Huang,Jie Chen
Renewable energy and electric vehicles are well-acknowledged strategies for reducing CO2 emissions, and their development relies heavily on the core of energy storage systems using lithium-ion batteries. However, recycling of lithium-ion batteries is far from mature, and massive abandonment of spent batteries would lead to severe environmental pollution. Meanwhile, the shortage of lithium resources brought about by the rapid development of lithium-ion batteries, especially LiFePO4, significantly drives up the preparation cost of Li4SiO4 as a promise sorbent and greatly limits its application as a CO2 capture scheme. Hence, a strategy is urgently needed to alleviate the lithium resource contradiction between energy storage and CO2 mitigation. Herein, we report a novel concept in recycling spent LiFePO4 battery to prepare high-efficiency and low-cost Li4SiO4 sorbents for CO2 capture. The obtained Li4SiO4 sorbents demonstrate very stable CO2 capacities of 0.27–0.28 g/g in a typical test up to 80 cycles, a leading level in CO2 capture, while the cost is only 1/6 of the conventional preparation process. It suggests that the concept of recycling spent LiFePO4 for CO2 capture has broad implications on resource utilization of energy waste and the mitigation of CO2 emissions.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xu Tang,Wenjing Shen,Dongyi Li,Binrong Li,Yemei Wang,Xianghai Song,Zhi Zhu,Pengwei Huo
The novel Co-doping combined with mesoporous g-C 3 N 4 -based photocatalyst was constructed, and the Co-CN showed impressive photocatalytic reduction CO 2 activity. Employing the DFT computation, we discussed the possible Co doping sites on g-C 3 N 4 framework, as well as the effects of band gaps, optical properties , and various densities of state (DOS) on photocatalytic activity. The adsorption energy calculation proved that the substitution and interstitial doping Co atoms in g-C 3 N 4 crystal unit cell was the stable configuration. The coexistence substitution and substitution the monolayer g-C 3 N 4 showed serious deformation. It indicated that the introduction of Co atoms leads g-C 3 N 4 molecular orbital redistribution and Co tends to occupy the conduction band, due to its weak electronegativity. Moreover, the DFT and experiment results pointed out that the doped-Co narrowed g-C 3 N 4 bandgap and increased light absorption from 450 to 800 nm, the improved charge carrier separation efficiency was originated from Co atom the unfilled 4 f and the empty 5d orbital act as electron capturing center. This research indicates the availability of transition metal g-C 3 N 4 with conducive photocatalytic activity.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yi Li,Yanghan Chen,Tao Chen,Guoqiang Shi,Lin Zhu,Ye Sun,Miao Yu
Ethanol (C2H5OH) is an economically ideal C2 product in electrochemical CO2 reduction. However, the CO2-to-C2H5OH conversion yield has been rather low and the underlying catalytic mechanism remains vague or unexplored in most cases. Herein, by decorating small Cu2S nanocrystals uniform ly on Cu nanosheets, three desirable features are integrated into the electrocatalyst, including a relatively high positive local charge on Cu (Cuδ+), abundant interfaces between Cuδ+ and zero-valence Cu0, and a non-flat, stepped catalyst surface, leading to the promoted affinity of *CO, decreased *COCO formation barrier, and thermodynamically preferred *CH2CHO-to-*CH3CHO conversion. As a result, a high partial current density of ∼20.7 mA cm–2 and a Faraday efficiency of 46% for C2H5OH are delivered at −1.2 V vs reversible hydrogen electrode in an H-cell containing a 0.1 M KHCO3 solution. This work proposes an efficient strategy for the high-yield CO2-to-C2H5OH conversion, emphasizing the promise for the industrial production of alcohol and related products from CO2.
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