ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xiaoqi Zhu,Lin Chen,Qisheng Fang,Jianli Cheng,Yuefeng Su,Paula Ratajczak,Francois Beguin,Bin Wang
Li-CO2 batteries with attractive characteristics of high energy density power supply and carbon dioxide fixation have attracted widespread attention. However, the lack of suitable cathode catalysts and their unsatisfactory electrochemical performance have impeded their development as promising Li-CO2 batteries for energy storage. Constructing heterojunctions by interfacial engineering to improve performance is considered one of the effective strategies. Herein, heterostructured CuCo2S4-Co9S8 nanosheets are fabricated by a facile hydrothermal method and employed as efficient cathode catalysts for Li-CO2 batteries. The construction of heterojunctions by interfacial engineering has proved as an effective strategy to enhance the electrochemical performance of the Li-CO2 batteries. The delocalized electrons between CuCo2S4 and Co9S8 contribute to a low median charge potential (∼3.6 V), small polarization (0.62 V), high energy efficiency of up to 83%, and outstanding cycle life (480 h) of the CuCo2S4-Co9S8 cathodes. Meanwhile, as a proof of concept, flexible fiber-shaped Li-CO2 batteries based on these cathodes are fabricated and demonstrate boosted flexibility adaptability and provide a stable power supply at various bending conditions.
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DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Jiaxi Yang,Dan Gao,Heng Zhang,Qun Yi
The efficient capture of carbon dioxide (CO 2 ) by porous ionic liquids (PILs) has become one of the important ways to deal with the greenhouse effect and enhance environmental protection. In order to enhance the CO 2 capture efficiency of PILs, 2 amino-functional ionic liquids (ILs) were synthesized in deionized water: tetraethylenepentamine-2-methylimidazole ([TEPA][MIm]) and diethylenetriamine-2-methylimidazole ([DETA][MIm]). 2 zeolite imidazolidin-8 frames (ZIF-8-W and ZIF-8-M) were prepared in methanol and deionized water. The performance of the material was verified through FT-IR infrared spectroscopy, TGA-DTG curves, XRD spectra, adsorption desorption curves, and corrosive changes. Based on this, the porous ionic liquid ZIF-8-W/[TEPA][MIm] with the best performance and ZIF-8-W with the best environmental friendliness were successfully constructed. The chemical reaction mechanism of CO 2 in PILs were explored. The results showed that the thermogravimetric temperature of all materials was greater than 370 K, and the difference in adsorption capacity between ZIF-8-W and ZIF-8-M was only about 36.3 ml/g, the maximum mass change rates of the two ILs after immersion in ceramic and stainless steel tubes for 7 days were only 0.78 % and 0.29 %, respectively. On the premise of ensuring fluidity, the maximum capture capacity of ZIF-8-W/[TEPA][MIm] for pure CO 2 reached 2.22 mol/mol PILs, and the maximum capture capacity for CO 2 in artificial flue gas reached 2.03 mol/mol PILs, which was 21.9 % and 31.6 % higher than the maximum capture capacity of pure ionic liquids, respectively. When [TEPA][MIm] in PILs reacts with CO 2 , it conforms to the characteristics of “zwitterions”.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ke Wang,Chuanjiang Yang,Pengfei Zhao,Edward J. Anthony
The addition of molten Na 2 CO 3 can drastically accelerated the extremely slow sorption kinetics of Li 4 SiO 4 -based CO 2 sorbents in the sorption enhanced reforming process. However, the lack of a unified consensus about the effect of doped Na 2 CO 3 on the CO 2 capture process, now delays the development of more-effective Li 4 SiO 4 sorbents. Here, sorption tests, sturactural characterzations and periodic density functional theory calculations were combined to develop a better mechanistic understanding CO 2 sorption on Na-doped Li 4 SiO 4 . The Na-doped Li 4 SiO 4 exhibited a better CO 2 capture performance than pure Li 4 SiO 4 even below the melting point of any eutectic mixtures. Structural characterizations revealed that rather than generating physical favorable characteristics, the Na doping substituted at the Li site and created lithium–sodium orthosilicates (Li 4-x Na x SiO 4 ). Theoretical calculations agreeing with experimental results further demonstrated that Li 4-x Na x SiO 4 presented a weaker Na-O bond and generated more active phases (quasi Li 2 O groups) for larger sorption energies, more charge transfers and stronger CO 3 2– bond formation, in turn providing more reactive sites for enhanced CO 2 chemisorption as comparing with pure Li 4 SiO 4 . Finally, we propose a new and unified sorption mechanism independent of the traditional “melting layer” explanation.
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DOI
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 40
·405201
·
IF 3.5
Zhuohua Chen,Xiaoli Jin,Qing Lan,Xin Li,Qunzeng Huang,Wenmin Liu,Yuwei Guo,Haiquan Xie,Liqun Ye
Photocatalytic CO2 reduction is considered to be an appealing way of alleviating environmental pollution and energy shortages simultaneously under mild condition. However, the activity is greatly limited by the poor separation of the photogenerated carriers. Ion doping is a feasible strategy to facilitate the charge transfer. In this work, Ni-doped Bi4O5I2 photocatalyst is successfully fabricated using a one-pot hydrothermal method. A few doping levels appear in the energy band of Bi4O5I2 after Ni doping, which are used as springboards for electrons transition, thus promoting photoexcited electrons and holes separation. As a consequence, a remarkably enhanced yield of CO and CH4 (6.2 and 1.9 μmol g−1 h−1) is obtained over the optimized Bi4O5I2-Ni15, which is approximately 2.1 and 3.8 times superior to pure Bi4O5I2, respectively. This work may serve as a model for the subsequent research of Bi-based photocatalysts to implement high-performance CO2 photoreduction.
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高影响因子
Nano Research
·
2024
·Vol. 17
·期 9
·7945-7956
·
IF 9.5
Li Ting,Zhang Zhen-Yu,Luo De-Cun,Xu Bo-Yu,Zhang Rong-Jiang,Yao Ji-Long,Li Dan,Xie Tao
Solar-driven photo-thermal catalytic CO 2 methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases emissions. However, designing advanced photo-thermal catalysts remains a research challenge for CO 2 methanation reaction. In this work, a series of ABO 3 (A = lanthanide, B = transition metal) perovskite catalysts with Ce-substituted LaNiO 3 (La 1− x Ce x NiO 3 , x = 0, 0.2, 0.5, 0.8, 1) were synthesized for CO 2 methanation. The La 0.2 Ce 0.8 NiO 3 exhibited the highest CH 4 formation rate of 258.9 mmol·g −1 ·h cat −1 , CO 2 conversion of 55.4% and 97.2% CH 4 selectivity at 300 °C with the light intensity of 2.9 W·cm −2 . Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties characterizations. The partial substitution of the A-site provided more active sites for the adsorption and activation of CO 2 /H 2 . The sources of the active sites were considered to be the oxygen vacancies (O v ) created by lattice distortions due to different species of ions (La 3+ , Ce 4+ , Ce 3+ ) and exsolved Ni 0 by H 2 reduction. The catalysts have excellent light absorption absorbance and low electron–hole (e − /h + ) recombination rate, which greatly contribute to the excellent performance in photo-thermal synergistic catalysis (PTC) CO 2 methanation. The results of in situ irradiated electron paramagnetic resonance spectrometer (ISI-EPR) and ISI-X-ray photoelectron spectroscopy (XPS) indicated that the aggregation of unpaired electrons near the defects and Ni metal (from La and Ce ions to O v and Ni 0 ) accelerated adsorption and activation of CO 2 /H 2 . At last, the catalyst properties and structure were correlated with the proposed reaction mechanism from the in situ diffuse reflection infrared Fourier transform spectrum (DRIFTS) measurements. The in situ precipitation of the B-site enhanced the dispersion of Ni, while its enriched photoelectrons upon illumination further promote hydrogen dissociation. More H* spillover accelerated the rate-determining step (RDS) of HCOO* hydrogenation. This work provides the theoretical basis for the development of catalysts and industrial application.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Songlin Wang,Nan Jiang,Jiali Peng,Peng Yang,Chengxing Cui,Hongying Niu,Qiying Zhang,Jianji Wang
Diphenyl carbonate (DPC) has outstanding practical potential, especially as a key building block for the phosgene-free synthesis of polycarbonate (PC) in the chemical industry. The synthesis of DPC from CO2 has been investigated for decades, but exploring highly efficient catalytic systems is still challenging. Herein, an efficient catalytic system for the direct synthesis of DPC from CO2, phenol, and carbon tetrachloride was developed by using a ZnCl2/copper triflate (Cu(OTf)2) composite catalyst. For the first time, high yield and high selectivity were achieved for DPC synthesis under mild conditions, even at atmospheric pressure. Carefully designed control experiments and DFT studies indicated that the synergistic activation of Cu(OTf)2 and its anion complex with ZnCl2 for phenol and CO2 led to a remarkably improved catalytic activity through a Lewis acid-assisted catalysis. This study not only provides a new strategy for efficient preparation of DPC but also offers an effective pathway for better CO2 utilization.
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DOI
高影响因子
Advanced Powder Materials
·
2026
·
IF 26.8
Minghao He,Zhenghui Tian,Rui Zhang,Yang Qu,Guofeng Wang
A B S T R A C T The key for photocatalytic CO 2 reduction in pure water lies in constructing active sites that possess both rapid charge transfer and efficient CO 2 adsorption. Here, atomically dysprosium (Dy)-cobalt (Co) dual sites anchored g-C 3 N 4 (CN) microtube were successfully fabricated by a precoordination-thermopolymerization strategy, in which Co 2+ and Dy 3+ ions are selectively coordinated with melamine and cyanuric acid, respectively, prior to thermal polymerization. The optimized Co 1 Dy 1 /CN catalyst delivers a CO yield of 240.55 μmol·g −1 and a CH 4 yield of 68.70 μmol·g -1 in pure water without sacrificial agents, representing ∼8.0-fold and ∼4.6-fold enhancements over pristine CN, respectively, superior to most reported single-atom photocatalysts. According to femtosecond transient absorption spectroscopy, theoretical calculation, and in situ techniques, the superior catalytic activity originates from the synergistic interaction between Dy and Co dual active sites. Specifically, Dy-possessing abundant unoccupied 4f orbitals-functions as an electron reservoir that facilitates directional electron transfer toward the Co sites, accelerating charge extraction by 8.4-fold and enhancing electron transfer kinetics by 1.5-fold. This electron enrichment at the Co centers induces a downshift in the Co d -band center, which further strengthens CO 2 adsorption and activation at the Co sites with inherent CO 2 affinity. In this paper, resent the lanthanide-empowered strategy to overcome charge dynamics limitations in cobalt single-atom catalysts. Dysprosium serves as an atomic electron reservoir adjacent to cobalt sites in dual sites centers, enabling synergistic CO2 reduction. Multimodal analysis (XAS, in situ spectroscopy, fs-TA, and DFT) reveals Dysprosium to cobalt electron transfer and d-band center optimization mechanisms. Download: Download high-res image (269KB) Download: Download full-size image
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2023
·Vol. 49
·期 9
·3933-3950
·
IF 3.3
Li Xiaojun,Xia Yudong,Xu Yangzhou,Li Haitao,Huang Jiangchao,Yao Jie,Zhao Heng,Gao Xinhua,Yu Jinghao,Guo Lisheng,Li Jie
Thermocatalytic conversion of redundant CO 2 to useful methanol is an attractive route to address both energy and environmental crises simultaneously. However, existing copper/oxide catalysts widely used in these thermocatalytic processes still suffer from low methanol yield under mild reaction conditions. In this work, we design inverse oxide/Cu catalysts to achieve superior thermal catalytic performance for CO 2 hydrogenation. The optimized ZnO/Cu-1.0 catalyst exhibits maximum CH 3 OH selectivity of 83.4% and space–time yield (STY) of \(170.9\;{\text{g}}_{{{\text{CH}}_{3} {\text{OH}}}} \;{\text{kg}}_{{{\text{cat}}}}^{ - 1} \;{\text{h}}^{ - 1}\) in CO 2 hydrogenation at 210 °C, nearly twofold higher STY than the previous optimal inverse ZnO/Cu catalysts ( \(89.6\;{\text{g}}_{{{\text{CH}}_{3} {\text{OH}}}} \;{\text{kg}}_{{{\text{cat}}}}^{ - 1} \;{\text{h}}^{ - 1}\) at 250 °C). Importantly, ZnO/Cu-1.0 catalyst displayed not only a satisfactory catalytic stability but also a superior CH 3 OH STY with a time-on-stream of 24 h. Such inverse configuration of catalysts will pave the way for new strategies to design high-performance thermocatalytic catalysts and promote their commercialization. Graphical abstract Typical inverse ZnO/Cu-1.0 catalysts have been demonstrated and achieved to significantly facilitate the activation of inert CO 2 molecules to produce methanol, due to its special physicochemical properties and strong ZnO–Cu interaction
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DOI
高影响因子
Journal of Physical Chemistry Letters
·
2023
·
IF 5.7
Qiang Huang,Chengfan Fu,Yangyi Shen,Haowen Wang,Zhengben Wu,Zhiyu Liang,Changqing Tian,Daofu Wu,Fei Qi,Yayun Pu,Nan Zhang,Manjing Wang,Xiaosheng Tang
Although dielectric barrier discharge (DBD) plasma is a promising technique for CO2 conversion, realizing CO2-to-alcohol is still challenging via the use of H2O. Herein, for the first time, efficient CO2 conversion was achieved via the synergism between the Cs2SnCl6 photocatalyst and DBD plasma assisted by H2O. The CO2 conversion ratio of plasma photocatalysis was 6.5% higher than that of only the plasma and photocatalysis, implying that the synergism of plasma catalysis and photocatalysis was achieved. Furthermore, the DBD plasma assisted by the Cs2SnCl6 photocatalyst could convert CO2 and H2O to CO and a small amount of methanol and ethanol. The CO2 conversion ratio was enhanced by 50.6% in the presence of H2O, which was attributed to the improvement of charge transfer due to the increased electrical conductivity of the photocatalyst surface during plasma discharge. This work provides a new idea for developing an efficient system for CO2 utilization.
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高影响因子
Nano Research
·
2024
·Vol. 17
·期 6
·5031-5039
·
IF 9.5
Li Wenxiang,Gao Shuo,Yang Chuanruo,Yang Juntao,Nisar Amjad,Xiang Guolei,Jin Junsu
In 2 O 3 is an effective electrocatalyst to convert CO 2 to formic acid (HCOOH), but its inherent poor electrical conductivity limits the efficient charge transfer during the reaction. Additionally, the tendency of In 2 O 3 particles to agglomerate during synthesis further limits the exposure of active sites. Here we address these issues by leveraging the template effect of graphene oxide and employing InBDC as a self-sacrificing template for the pyrolysis synthesis of In 2 O 3 @C. The resulting In 2 O 3 @C/rGO-600 material features In 2 O 3 @C nanocubes uniformly anchored on a support of reduced graphene oxide (rGO), significantly enhancing the active sites exposure. The conductive rGO network facilitates charge transfer during electrocatalysis, and the presence of oxygen vacancies generated during pyrolysis, combined with the strong electron-donating ability of rGO, enhances the adsorption and activation of CO 2 . In performance evaluation, In 2 O 3 @C/rGO-600 exhibits a remarkable HCOOH Faradaic efficiency exceeding 94.0% over a broad potential window of −0.7 to −1.0 V (vs. reversible hydrogen electrode (RHE)), with the highest value of 97.9% at −0.9 V (vs. RHE) in a H-cell. Moreover, the material demonstrates an excellent cathodic energy efficiency of 71.6% at −0.7 V (vs. RHE). The study underscores the efficacy of uniformly anchoring metal oxide nanoparticles onto rGO for enhancing the electrocatalytic CO 2 reduction performance of materials.
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高影响因子
ARABIAN JOURNAL FOR SCIENCE AND ENGINEERING
·
2024
·Vol. 50
·期 13
·10327-10344
·
IF 2.6
Xu Ruifeng,Wang Shuoshi,Guo Ping,Hukuang Haoxiang,Yuan Na
The CO 2 -WAG injection method proposed for unconventional tight oil reservoirs has been successfully applied in field. However, for water-sensitive tight oil reservoirs, there is a lack of research focusing on the displacement mechanisms and effects of WAG injection at the pore scale. And the gap between nuclear magnetic resonance (NMR) and computerized tomography (CT) scanning technologies is not well explored. This study integrated deuterium oxide-shielded NMR and contrast agent (n-butane iodide and lead iso-octanoate mixture) enhanced micro-CT to study the immiscible CO 2 -WAG mechanisms for water-sensitive tight oil. The aim is to investigate the microscopic distribution and displacement mechanisms of residual oil after CO 2 flooding and WAG injection in water-sensitive cores. Experimental results showed that NMR experiments and CT experiments identified the microscopic distribution of oil at different injection stages successfully. The contrast agent, despite its similar viscosity ratio, had poor representativeness in other properties, leading to significant differences in the microscopic fluid distribution results compared to NMR experiments. The primary WAG flood mechanism observed was that CO 2 dispersed oil droplets, with most being displaced out of the pores, while water played a mobility control role by blocking large pores. However, due to water sensitivity, medium and small pores also experienced blockage, making the effect of WAG injection after CO 2 flooding not significant. In the NMR experiment, the final recovery of core 6–1 after WAG injection was 64.71%. In the CT scan experiment, due to the smaller volume of the microcore, the water sensitivity effect was relatively weaker, and under the stronger influence of the capillary end effect, the final recovery reached 76.91%. In the five sets of long-core experiments, by controlling the gas–water ratio and slug size, the recovery ranged from 56.51 to 64.04%. The core flood experiments validated the representativeness of the microscopic experiments. And for water-sensitive tight oil reservoirs, controlling the volumes of water and CO 2 during the WAG injection process is crucial.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ming-Long Wang,Yi-Fei Sun,Hong-Nan Chen,Jin-Rong Zhong,Dan Rao,Yu Liu,De-Jun Xuan,Bei Liu,Chang-Yu Sun,Guang-Jin Chen
The CO 2 -H 2 O emulsion has multiple advantages in forming hydrate, such as easily adjustable CO 2 -to-H 2 O ratio, large contact area, strong sweep efficiency, and ability to carry chemical agents, which holds great promise for large-scale solid CO 2 geological sequestration. This paper systematically investigates the kinetics of hydrate formation from CO 2 -H 2 O emulsion and the corresponding morphological features in glass beads under different pore sizes at 3.27–7.15 °C and 10–14 MPa. Quantitative results on CO 2 hydrate formation rates, quantities, conversion rates, and hydrate saturations are obtained. Overall, under multi-factors, the conversion rates of CO 2 hydrate range from 22.9 % to 56.3 %, and hydrate saturations range from 18.5 % to 45.4 %. Here, lower temperature and higher pressure can enhance hydrate formation and increase the final conversion rate. As the pore size decreases, CO 2 hydrate conversion ratio increases, but the formation rate shows a significant decline. Additionally, under flowing conditions, hydrate conversion rates are further increased to 44.4 %–76.5 %, and its enhancement mechanism has been observed and revealed. Even though CO 2 droplets remain spatially separated, hydrate formation still demonstrates remarkably rapid propagation. These results prove the potential of CO 2 emulsion as an excellent medium for CO 2 hydrate storage and provide a direction for more effective carbon storage.
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