ENERGY & FUELS
·
2025
·
IF 5.3
Yang Li,Xiaodong Shen,Xinlei Shi,Nanqin Zhou,Yinde Zhang,Bo Wang
Hydrate-based CO2 sequestration in submarine sediments is a promising large-scale carbon mitigation strategy. This study examined the effects of sediment grain size on CO2 hydrate formation kinetics, seepage behavior, and morphology evolution regulated by l-Methionine (l-Met) as a kinetic promoter, under controlled conditions of 3.6 MPa and 277.15 K, simulating the harsh environment of submarine organic-rich sediments. The experimental results demonstrate a nonunidirectional relationship between grain size reduction and sequestration enhancement. While finer sediments generally promote formation kinetics, the 98–138 μm quartz sand fraction exhibited optimal overall performance, achieving a CO2 consumption of 0.369 mol and the fastest growth rate (t90 = 58.027 min). This optimum reflects a balance between kinetic promotion and mass transfer, as evidenced by seepage tests showing that excessively fine sediments cause severe pore-throat clogging, leading to a marked reduction in effective permeability, whereas medium-grained systems exhibit the highest effective permeability. Mixed-grain systems display enhanced injectivity due to preferential flow pathways formed by coarse fractions. Visual observations reveal that CO2 hydrate in natural sea sands forms heterogeneously with nodular-like morphology. These findings offer theoretical guidance for optimizing kinetic promoter-regulated CO2 hydrate formation and continuous CO2 injection strategies in submarine sediments.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Xi Chen,Nana Wang,Guining Chen,Zhenggang Wang,Gongping Liu,Rongfei Zhou,Wanqin Jin
Mixed-matrix formulation is a promising method to overcome permeability-selectivity trade-off of polymers with incorporation of fillers with well-defined nanopores . The filler properties play a key role in determining the performance of mixed-matrix membrane (MMM). In this work, for the first time, we explored the critical effect of filler structural integrity on separation performance of MMM. Typically, micron as-synthesized, submicron as-synthesized and submicron ground SAPO-34 zeolites were incorporated into 6FDA-DAM polyimide , respectively. The interface compatibility between two phases was ensured by (3-aminopropyl) trimethoxysilane (APTMS) modification on SAPO-34 fillers. It was found that the directly synthesized micron and submicron fillers contributed to enhance the CO 2 /CH 4 separation performance whereas the submicron ground filler lowered the CO 2 permeability. Notably, incorporating 30 wt% micron as-synthesized SAPO-34 into 6FDA-DAM enhanced the CO 2 permeability by 68% and CO 2 /CH 4 by 37%, surpassing the performance upper-bound. Moreover, the hydrogen bonding between the filler and polymer matrix endowed the membrane with outstanding plasticization resistance with CO 2 partial pressure up to 20 bar. Adsorption isotherms and Maxwell model prediction revealed that the filler transport properties could be significantly affected by commonly-used methods of reducing the filler size. A decreased structural integrity was identified in the sequence of micron as-synthesized, submicron as-synthesized and submicron ground fillers. This work highlights the importance of a careful balance between structural integrity and crystal size of filler, and reliable routes to obtain nanofillers with desirable structural integrity as pursuing high-performing MMM toward practical application.
研究领域:
材料科学
·
化学工程
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ENERGY
·
2020
·
IF 6.082
Hongwei Li,Zhigang Tang,Zhimin He,Xia Gui,Longpeng Cui,Xian-zhong Mao
In order to show the structure-activity relationship for CO 2 absorbent, and identify or screen novel and efficient physical solvents of CO 2 , the constant-volume method, the Peng-Robinson equation of state , and a molecular simulation were used to investigate the impacts of type of functional groups, carbon chain length and number of functional groups for nine physical solvents. The three methods produced highly consistent results. Comparison of the CO 2 solubility in solvents with the same carbon numbers but different functional groups suggested that the ester group could promote CO 2 absorption. Investigation of the CO 2 solubility in solvents with one ester group but different carbon chain lengths revealed that longer carbon chains could enhance CO 2 absorption. Analyses of the CO 2 solubility of solvents with one and two ester groups demonstrated that more ester groups could further increase the CO 2 absorption. Therefore, the presence and number of ester groups and increased carbon chain length could promote CO 2 absorption. It provides direction and method for screening of highly efficient CO 2 absorbents and for the design and synthesis of new solvents.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Liu Tao,Wang Yunpeng,Wu Yifan,Jiang Wenchuan,Deng Yuchao,Li Qing,Lan Cheng,Zhao Zhiyu,Zhu Liangyu,Yang Dongsheng,Noël Timothy,Xie Heping
Electrochemical CO 2 capture driven by renewable electricity holds significant potential for efficient decarbonization. However, the widespread adoption of this approach is currently limited by issues such as instability, discontinuity, high energy demand, and challenges in scaling up. In this study, we propose a scalable strategy that addresses these limitations by transforming the conventional single-step electrochemical redox reaction into a stepwise electrochemical-chemical redox process. Specifically, the hydrogen evolution reaction (HER) at the cathode and the oxidation of a redox carrier at the anode are employed to modulate the pH of the electrolyte, thereby facilitating effective CO 2 capture. By decoupling the electrochemical swing for CO 2 capture from redox carrier regeneration in both temporal and spatial domains, this approach mitigates unwanted side reactions and enhances system stability. Our results demonstrate a stable CO 2 capture process sustained for over 200 h, with a electrical work of 49.16 kJ e mol -1 CO 2 at a current density of 10 mA cm -2 . Furthermore, a scaled-up system capable of producing approximately 0.4 kg of pure CO 2 per day maintained stable operation for 72 h, highlighting the potential feasibility of this method for large-scale decarbonization applications.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-8
·
IF 15.7
Zhang Zhewei,Yao Jun,Shen Chenyang,Li Fengfeng,Deng Changshun,Zhao Taotao,Guo Xuefeng,Zhu Yan,Guo Xiangke,Xue Nianhua,Peng Luming,Ding Weiping
In typical heterogeneous catalytic reactions, catalysts, whether fixed or flowing, maintained their bulk and surface structures as stable as possible. We report here dynamic activation catalysts having continuously generate highly active sites in working, which enables a usually low active Cu/Al 2 O 3 catalyst for CO 2 hydrogenation, showing extraordinary catalytic performances. Using reaction streams in unusually high linear speed to blow and carry the Cu/Al 2 O 3 particulates to collide cyclically with a rigid target, the CO 2 conversion rate is more than three times enhanced at methanol selectivity promoted to 95% from less than 40% and the methanol space-time-yield is six times increased. By experimental and theoretical investigation, the dynamic activation of Cu/Al 2 O 3 is defined as a discrete condensed state with a distorted and elongated lattice, reduced coordination, and abnormal catalytic properties. We envision that continuous research on the dynamical activation catalysts will advance novel methods for promoting catalytic performance and discovering new catalytic reactions.
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RSC Advances
·
2023
·Vol. 13
·期 20
·13902-13910
·
IF 3.9
Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying
In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.
研究领域:
催化
·
化学工程
·
材料科学
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ENERGY & FUELS
·
2017
·
IF 3.091
Yingchao Hu,Wenqiang Liu,Zijian Zhou,Yuandong Yang
Various synthesis methods, such as the combustion method, sol–gel method, impregnated suspension, precipitation, etc., have been previously proposed for the production of efficient Li4SiO4 sorbents. During these methods, the mixture of the precursors of Li and Si were usually dried through the oven, water bath, or oil bath, which are all energy-consuming and slow processes. To produce Li4SiO4 sorbents quickly and efficiently, the spray-drying technique was employed in this work. The spray-dried sorbents exhibited both excellent CO2 capture capacity and cyclic stability during the multiple cycles, indicating that the spray-drying method was effective for the preparation of efficient and durable Li4SiO4 sorbents for high-temperature CO2 removal. Especially, the sorbent using lithium tartrate as the Li source achieved a considerable first-cycle CO2 sorption capacity of ∼0.275 g of CO2/g of sorbent and still held the capacity of ∼0.248 at the 50th sorption/desorption cycle under the realistically low CO2 concentration of 15 vol %. The excellent performance of the sorbent was demonstrated to be attributed to the corresponding small crystallite size of Li4SiO4, high surface area, large pore volume, and rich porosity.
研究领域:
材料科学
·
环境科学
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JOURNAL OF MEMBRANE SCIENCE
·
2017
·
IF 6.035
Xingyu Wu,Wei Liu,Hong Wu,Xue Zong,Leixin Yang,Yingzhen Wu,Yanxiong Ren,Chengyou Shi,Shaofei Wang,Zhongyi Jiang
In this study, novel kinds of MMMs were fabricated by incorporating ZIF-67 nanoparticles into polymers of intrinsic microporosity (PIM-1). ZIF-67 (Co substituted ZIF-8) displays stiffer Co-N bond as compared with the Zn-N bond in ZIF-8, which might led to the slightly smaller effective pore aperture of ZIF-67. Good compatibility between ZIF-67 nanoparticles and PIM-1 matrix rendered ideal interfacial morphology. The intrinsic separation performance of ZIF-67 was estimated from our experimental separation results based on the Maxwell model. The calculation demonstrated its superior CO 2 /CH 4 selectivity of 45, which is twice compared with that of ZIF-8, supporting the high molecular sieving efficiency of PIM-1/ZIF-67 MMMs. Particularly, the CO 2 and H 2 permeability increased by 15.1% and 59.6% for PIM-1 membrane with 20 wt% ZIF-67 loading, meanwhile CO 2 /CH 4 and H 2 /CH 4 selectivity increased by 34.4% and 86.96%, respectively. The strategy of incorporating highly selective ZIFs into polymers of intrinsic microporosity may have promising potential in fabricating high performance membranes for efficient gas separation.
研究领域:
材料科学
·
化学工程
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Nano Research
·
2023
·Vol. 17
·期 5
·3684-3692
·
IF 9.9
Wu Wenbo,Zhu Jiaye,Tong Yun,Xiang Shuangfei,Chen Pengzuo
Regulating the electronic structure of Bi-based materials by alloying engineering is promising to promote the electrocatalytic activity, but it remains some challenges to be solved. In this study, a facile electrochemical co-deposition strategy is developed to synthesize the bimetallic Bi 9 Cu 1 alloy nanosheet on carbon cloth (Bi 9 Cu 1 /CC), which represents a novel self-supporting electrode for the electrocatalytic carbon dioxide (CO 2 ) reduction reaction (CO 2 RR). The Bi 9 Cu 1 /CC catalyst has achieved a remarkable catalytic performance with high Faradaic efficiencies (FE) of over 90% for formate at wide potentials from −0.7 to −1.2 V vs. reversible hydrogen electrode (RHE). Moreover, the reversible Zn-CO 2 battery can be driven by Bi 9 Cu 1 /CC cathode with a largest power density of 1.4 mW·cm −2 , and superior operating stability. The systematic characterizations and electrochemical results confirm that the improved catalytic active sites, the enhanced mass/charge transport and the optimal reaction kinetics of Bi nanosheet are realized for CO 2 RR by Cu alloying. In situ attenuated total reflection infrared (ATR-IR) result confirms the bimetallic Bi-Cu active sites prefer to follow the ⋆OCHO conversion pathway. The density functional theory (DFT) calculations suggest that the Cu alloying contributes to the increased density of states near the Fermi surface of Bi and the optimized adsorption of ⋆OCHO intermediates on the Bi sites, resulting in the excellent catalytic performance.
研究领域:
材料科学
·
电化学
·
能源存储与转换
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LANGMUIR
·
2026
·Vol. 42
·期 31
·22950-22957
·
IF 4.4
Chen Nannan,Yuan Qingle,Liu Qin,Zhang Chao,Wu Zhengcui,Bi Wentuan
Single-atom catalysts (SACs) hold great promise for the
electrochemical
reduction of CO 2 to CO; however, the high selectivity is
typically restricted within a narrow potential window, limiting their
practical implementation. In this study, Ni–N–C catalysts
were supported on ordered and disordered carbon nanofiber membranes
(denoted as o-NiNC and d-NiNC, respectively) via electrospinning to
elucidate the effect of nanofiber alignment on CO 2 reduction
activity. The results demonstrate that o-NiNC catalysts allow for
spatially uniform H + /CO 2 delivery and consumption,
thereby mitigating the selectivity variations arising from uneven
spatial distribution of reactants. As a result, the o-NiNC catalysts
achieve a CO Faradaic efficiency (FE) of 98.5% at −1.0 V and
maintain an FE above 90% across a broad potential range (−0.6
to −1.6 V). This work provides new insights into the rational
design of high-performance CO 2 reduction electrocatalysts
through geometric engineering.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yang Chen,Pengfei Yan,Huanhuan Yang,Huan He,Huiwen Tian,Xueqi Liu,Jingjing Zhang,Huimin Lv,Wenzhuo Wu,Qun Xu,Buxing Han
Supercritical CO 2 works as a soft oxidant to adjust the oxidation states and crystal facets of Cu-based materials. • In the supercritical state, CO 2 dissociates to generate active *O on the Cu surface with water assistance. • Spontaneously reconstructed hydrogen bond network stabilizes the dissociated *O species for Cu oxidation to Cu 2 O {111}. • Ethanol induces thermodynamic selectivity towards Cu 2 O {110} facets via an interfacial adsorption coupling mechanism. • Facet-engineered Cu 2 O-Cu achieves over 73% Faradaic efficiency for CO 2 RR-to-syngas and a tunable CO/H 2 ratio of 0.25−0.94. Catalytic versatility of copper-based catalysts has been demonstrated to arise from synergistic effect between Cu and Cu 2 O with controlled crystal facets, though precise synthesis of crystal facet-tailored Cu-based catalysts remains challenging. Herein, we develop a novel strategy to partially convert Cu nanoparticles into crystallographically defined Cu 2 O with supercritical CO 2 (scCO 2 ) as soft oxidant. Under supercritical fluid state, CO 2 dissociation on Cu surface generates reactive ⁎ O species with assistance of water. The spontaneously reconstructed hydrogen bond network with surrounding water molecules stabilizes these dissociated ⁎ O species for Cu oxidation to Cu 2 O with exposure of {111} crystal facet. While, ethanol introduction induces the formation of Cu 2 O {110} rather than Cu 2 O {111} facet from a thermodynamic perspective through interfacial adsorption coupling. The resulting facet-engineered Cu 2 O-Cu catalysts exhibit excellent electrochemical CO 2 reduction reaction (CO 2 RR) for syngas production with a high Faradaic efficiency of >73% and a tunable CO/H 2 ratio of 0.25–0.94. The enhanced performance is attributed to the interfacial synergy between Cu and Cu 2 O with distinct crystal facets, which facilitates significantly improved electron transfer to the key ⁎ COOH intermediate and thus lowers the energy barrier for CO formation. This interfacial effect is particularly pronounced in Cu/Cu 2 O {110}. This scalable platform enables solvent-directed synthesis of surface-customized metal oxides for functional nanomaterials using scCO 2 as mild oxidant. Supercritical CO 2 dissociates to active ⁎ O species for Cu oxidation to Cu 2 O {111} with assistance of water, while ethanol introduction induces Cu 2 O {110} formation. The face-engineered Cu 2 O-Cu demonstrated enhanced CO 2 RR-to-syngas performance. Download: Download high-res image (92KB) Download: Download full-size image
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Nanomaterials
·
2026
·Vol. 16
·期 8
·489
·
IF 4.8
Xin Peng,Lina Du,Gaoliang Fu,Shouren Zhang,Junying Ma
Photocatalytic reduction of carbon dioxide (CO2) into high-value multicarbon products, such as ethylene (C2H4), remains a significant challenge due to the difficult C-C coupling process. Potassium poly(heptazine imide) (K-PHI) is a promising photocatalyst, yet efficiently exchanging its interlayer cations to tune catalytic selectivity without causing structural degradation is difficult. Herein, an efficient and green supercritical CO2(SC CO2) assisted ion-exchange strategy was developed to successfully prepare a series of mono-/di-/trivalent cation-doped M-PHI photocatalysts (M = H+, Na+, Sr+, Ca2+, Co2+, Fe3+). Systematic characterizations confirmed that the SC-CO2treatment successfully achieved in-depth cation substitution without destroying the intrinsic heptazine framework, effectively regulating the interlayer structure and significantly optimizing the photoelectrochemical charge separation. Among the prepared samples, H-PHI exhibited the optimal photocatalytic CO2reduction performance with an outstanding selectivity toward C2H4generation. Under simulated sunlight irradiation for 3 h, the yields of CO, CH4, and C2H4C2H4C2H4reached 3564.87, 807.32, and 40.00 μmol·g−1, respectively, significantly outperforming pristine K-PHI and other metal-doped samples. Crucially, isotope-tracing experiments utilizing a SC CO2-DCl treatment detected deuterated CH4and C2H4products, providing direct evidence that the hydrogen in the carbon products originates from the introduced protons, thereby elucidating the precise reaction pathway for C-C coupling. This study provides a green and efficient supercritical CO2ion exchange strategy for the cation engineering of crystalline carbon nitride, and also offers new ideas and methods for designing high-activity photocatalysts for photocatalytic CO2reduction.
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