JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Ajibola T. Ogunbiyi,Wenzhi Li,Amir Hamza,Chenchen Gui,Liqun Wang
Despite significant advances in lignin depolymerization studies, the specific combination of Mo and W in bimetallic catalysts and their impact on hydrogen activation and Lewis acidity in lignin conversion remains poorly understood, particularly in terms of the synergistic effects that enhance efficiency and selectivity. A bimetallic Mo x W y /H-Beta catalyst was synthesized via incipient wetness impregnation with the catalyst characterized using XPS, H 2 -TPR, NH 3 -TPD, and other methods. The catalyst demonstrated high activity for selective kraft lignin depolymerization due to the synergy between Lewis acid sites, hydrogen activation sites, and the Mo-W interaction on the support. The proximity of metal and acid sites facilitated effective diffusion of intermediates, leading to enhanced synergy and the eventual cleavage of etheric C–O bonds. A Liquid fuel (LF) yield of 84.3 % and 71.6 % kraft lignin conversion at 300 °C without external hydrogen. The higher heating value (HHV) increased from 25.45 MJ/kg in the original kraft lignin feed to 35.9 MJ/kg in the LF. XPS analysis showed a predominant amount of Mo 6+ on the fresh catalyst surface, with complete conversion to lower oxidation states during the reaction. This study provides insights into the structure–activity relationships of Mo-based bimetallic catalysts, highlighting the importance of hydrogen activation sites and acidic sites in kraft lignin depolymerization.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Jinwei Zhang,Yujun Zhang,Ning Li,Shilin Nie,Leixin Yang,Yihao Luan,Yuchao Ma,Ge Wang,Kaihua Li,Long Jiao,Bowen Cheng
Physical aging presents a significant challenge that hinders the practical application of high-permeability polymer-based membranes. Herein, we have designed a polymer network membrane (PI–CO@Trip-TB (1:10)) featuring H-bonding interactions by regulating the ratio of the carboxyl-containing copolymer PI-CO (6FDA-FDA-DABA) to Trip-TB (Tröger's base), which significantly improved the anti-aging performance without compromising the high permeability. The introduction of PI-CO not only generates H-bonding interactions to enhance compatibility, but also the introduction of its linear chain segments effectively hinders the relaxation of the chain of the Trip-TB spatial structure. Which synergistically stabilizes the free volume elements and mitigates the rate of their temporal collapse. Compared to Trip-TB, the PI-CO@Trip-TB (1:10) polymer network membrane demonstrates outstanding anti-aging performance, in which the permeability of CO 2 and O 2 is maintained at approximately 60 % even after 90 days. Notably, the performance of both fresh and aged PI-CO@Trip-TB (1:10) membranes surpasses the 2008 Robeson upper bound (CO 2 /CH 4 ) and the 2015 Robeson upper bound (O 2 /N 2 ). Overall, this study establishes an effective strategy for designing high-permeability polymers with anti-aging properties for practical applications in separation membranes.
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Materials Today Communications
·
2025
·
IF 4.5
Chengzhen Fu,Hailu Wang,Hongxing Zhan,Yuanbing Li,Shujing Li,Bo Yin
Reducing the Ca/Si molar ratio is critical for optimizing calcium silicate hydrate (C–S–H) materials and enabling the recycling of silicon-rich waste. However, achieving high-performance crystalline C–S–H at Ca/Si < 0.83 remains challenging. This study proposes and systematically investigates a dual-silicon-source strategy, employing both active and inert silicon sources to regulate hydrothermal synthesis. At Ca/Si = 0.6, experimental results demonstrate that increasing the active silicon source content from 0 % to 60 % enhances tobermorite crystallinity by 275 %, decreases thermal conductivity by 26 %, and improves compressive strength by 7.30 MPa. The optimal performance was obtained at a reactive silicon-to-calcium molar ratio of 1.0. These findings confirm that this strategy significantly enhances C–S–H crystallinity and material performance. Mechanistically, the higher reactivity of the active silicon source drives competitive calcium consumption, facilitating the formation of long-chain crystalline C–S–H. This approach demonstrates a scalable pathway for synthesizing high-performance C–S–H under low Ca/Si conditions, offering promising applications in optimizing C–S–H-based materials and the recycling of silicon-rich waste.
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Molecular Catalysis
·
2025
·
IF 4.9
Shan Lin,Haiyang Xu,Shengjie Wei,Zheng Zhou,Xu Zhang,Xuan Tong,Hangyu Zhou,Xiaodong Ma,Xu Ji,Yue Yang,Le Zhang
To enhance the hydrogen production performance and photo-corrosion resistance of ZnS and CdS based photocatalysts without relying on noble metals such as platinum, ruthenium, or gold, this study optimizes the molar ratio between Cd and Zn in Zn x Cd 1-x S solid solutions. The resulting Zn 0.4 Cd 0.6 S nanorod-shaped solid solutions exhibit superior visible-light photocatalytic activity. A non-precious metal Ni 3 (PO 4 ) 2 nano-thin layer is uniformly deposited onto the surface of the Zn 0.4 Cd 0.6 S solid solution via a room-temperature chemical co-precipitation method. This modification not only prevents oxidative photo-corrosion but also facilitates the oxidation and reduction of water during the photocatalytic surface process, significantly enhancing both the stability and hydrogen production performance of the composite catalyst. Experimental results demonstrate that the performance improvement of Zn 0.4 Cd 0.6 S by the Ni 3 (PO 4 ) 2 cocatalyst is markedly greater than that achieved with the traditional Pt cocatalyst. The maximum hydrogen production rate of the composite catalyst reaches 119.72 mmol·g⁻¹·h⁻¹, with an accumulated hydrogen production of 340.33 mmol·g⁻¹ after 3 hours. After 25 hours of photocatalytic cycling experiments, the hydrogen production rate remains at 95.95 mmol·g⁻¹·h⁻¹, approximately 80.14 % of the initial rate. The apparent quantum yield of Z4C6S-5NPO attains 61.8 %, with high value in ZnCdS-based photocatalysts. These results are promising and offer valuable insights for the development of low-cost, highly stable, and efficient composite photocatalysts.
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COMPOSITE STRUCTURES
·
2025
·
IF 7.1
Fan Xie,Qiaoling Liu,Longhai Zhuo,Haitao Wei,Yuxuan Shang,Tao Liu,Zhaoqing Lu
High-performance electromagnetic interference (EMI) shielding materials with lightweight, multi-resistant properties and superior, tunable EMI shielding performance are urgently needed for next-generation integrated electronic and communication systems, particularly in portable smart devices and artificial intelligence applications. In this work, hollow h-MXene/ANF backbones with a continuous shielding network were fabricated using a facile vacuum-assisted filtration process combined with a sacrificial template method. The structurally engineered h-MXene/ANF hybrid films achieved outstanding EMI shielding effectiveness (EMI SE) of 78.9 dB and EMI specific shielding effectiveness per unit thickness (SSE/t) of 15703 dB·cm 2 ·g –1 . These exceptional properties are attributed to high ohmic losses, multiple internal reflections, polarization relaxation, and efficient losses in the hollow MXene conductive layer, facilitated by impedance mismatches within the sandwich structure. Notably, the EMI SE performance can be tuned by adjusting the content of hollow MXene microspheres. In addition, extensive hydrogen-bonding interactions between the high-performance ANF and MXene contribute to enhanced mechanical properties, including tensile strength of up to 37 MPa, as well as excellent thermal stability and self-cleaning capabilities. Overall, the sandwich-structured h-MXene/ANF hybrid films exhibit superior mechanical strength, multi-resistant properties, and ultra-high, tunable EMI shielding performance, making them promising candidates for advanced EMI shielding in next-generation portable smart electronic devices.
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CEMENT AND CONCRETE RESEARCH
·
2025
·
IF 13.1
Haochuan Wang,Xin Liu,Chong Wang,Wei Wang,Jinxiang Hong,Pan Feng
Ultra-early mechanical properties are critical for shotcrete performance, significantly influenced by ettringite and calcium silicate hydrate (C-S-H) formed during the initial hydration stage and free water. This study investigates the individual and synergistic effects of these phases on mechanical behavior using equivalent cement pastes. In this system, cement was entirely replaced with dolomite particles of matching size distribution, with the controlled introduction of free water, ettringite, and C-S-H. The validity of these equivalent systems was confirmed through comprehensive characterization. Mechanical performance was subsequently evaluated using compression, shear, Vickers hardness and nanoindentation tests. Results revealed that free water remarkably weakened the mechanical properties, whereas both ettringite and C-S-H enhanced strength by reducing voids and reinforcing weak particle interfaces. Ettringite primarily contributed to interparticle friction, while C-S-H enhanced cohesion at interfaces including dolomite-dolomite, dolomite-ettringite and ettringite-ettringite contacts. When co-existing, C-S-H formed within the porous ettringite network, not only establishing a multi-scale filling structure but also stabilizing the dolomite-ettringite skeleton. These findings advance our understanding of the early-age mechanical development of shotcrete and highlight the potential of equivalent cement systems as robust tools for research into cementitious materials.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Jun Tu,Qiuru Chen,Siyu Ke,Xiaohui Yi,Yiquan Qiu,Ziyi Lin,Shuxiang Yang,Xinzhi Wang,Xiaotong Bai,Mingzhi Huang
In this study, corn stover biochar was prepared and modified with manganese (II) chloride (MnCl 2 ) and phosphoric acid (H 3 PO 4 ) to investigate the adsorption performance and mechanism of neonicotinoids represented by clothianidin (CLO). MnCl 2 promotes pore formation in biomass and enhances activation efficiency, while H 3 PO 4 boosts the specific surface area and adsorption capacity of the product. These properties make them widely used in biomass activation. The modified biochar (Mn-P-BC) exhibited an adsorption capacity of 11.5 mg·L -1 for CLO, representing a 2.8-fold enhancement compared to unmodified biochar (BC). In materials characterization, SEM and BET analysis results show that Mn-P-BC has a developed porous structure, and the surface area increases by 13.7 times compared with BC, which can provide more adsorption sites. According to the electrochemical properties, kinetics, and isotherm analyses, the adsorption mechanism for CLO was identified as involving physicochemical processes. Furthermore, density functional theory (DFT) calculations indicated that Mn-P-BC was more efficient in removing CLO compared to thiamethoxam (THM) and imidacloprid (IMI). It is shown that the mechanism of interaction between Mn-P-BC and CLO mainly involves pore filling, π-π interactions, and hydrogen bonding. In summary, the co-modification of biochar with MnCl 2 and H₃PO₄ significantly improved the adsorption performance of biochar, which provided new insights into the development of adsorbents for neonicotinoid insecticide removal.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
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IF 4.8
Tianyu Bai,Jinquan Tao,Yijing Jia,Wenbin Huang,Rongpeng Yao,Xinan Xue,Yasong Zhou,Qiang Wei
In the research of directly synthesizing H-form ZSM-5, ammonium hydroxide is commonly used as an alkali source instead of NaOH to avoid multiple ion exchange steps. However, the volatile nature and the lack of structure-directing effect of ammonium hydroxide limit its application in practical. In this study, n -butylamine (NBA) was used as the main alkali source to directly prepare HZSM-5 zeolites with SiO 2 /Al 2 O 3 ratios ranging from 40 to 300 under traditional hydrothermal conditions. The influence of the amount of NBA, ethanol, seed, and pre-crystallization on the synthesis products was investigated under the condition of SiO 2 /Al 2 O 3 = 80. Theoretical simulation suggested that n -butylamine cations (NBA + ) play the most potent directing role in the formation of the MFI structure but could lead to difficulties in removal during calcination. The addition of ethanol as the zeolite growth modifier (ZGM) could decrease the usage of NBA and reduce the difficulties in calcination, and the addition of seed provided the conditions for initiating crystallization in the system that could not spontaneously nucleate. HZSM-5 with different SiO 2 /Al 2 O 3 ratios were prepared under the optimal crystallization conditions, and the as-synthesized samples exhibited superior textural and acid properties compared to commercial zeolite. Finally, the 1 L scale-up synthesis and MTP reaction were conducted to demonstrate the practicality of this economically and environmentally-friendly synthesis strategy.
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Sustainable Energy & Fuels
·
2021
·Vol. 6
·期 2
·440-448
·
IF 6.367
Xin Liang,Lulu Wang,Yang Wang,Yongchao Liu,Yi Sun,Hongfa Xiang
The functional design of separators has been proved to be one of the most efficient methods to improve the electrochemical performance of lithium–sulfur batteries. In this work, a multifunctional separator with gradual changes to four aspects was constructed by integrating a PVDF-HFP/h-BN membrane with a Co-doped carbon nanofiber. The architecture has four gradations, which offers multifold advantages. First, in terms of density, there is a transition from loose to dense, which results in a higher electrolyte uptake rate, reduces the amount of free electrolyte and further suppresses the shuttle effect. Additionally, in terms of composition, a transition from inorganic to organic is designed, which allows the inorganic and organic components to bind closely and reduces the interfacial resistance. Meanwhile, there is a transition from high electronic conductivity to insulation. The change in electronic conductivity leads to effective conversion of the polysulfide. Finally, in terms of ionic conductivity, there is a transition from low to high, which gives the separator better ability to conduct lithium ions. As a consequence, a battery with the as-constructed multifunctional separator performs with good capacity stability, which demonstrates a new concept for high-performance lithium–sulfur battery design.
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Energetic Materials Frontiers
·
2022
·
IF 0
Zhi-qiang Wang,Zhen-qi Zhang,Shan-hu Sun,Mi Yan,Shi-liang Huang,Shuang-qi Hu,Jin-jiang Xu,Li-shuang Hu
Polymorphs of energetic materials generally exhibit distinct features, such as density, thermal stability, sensitivity, and detonation performance. These features are important in determining the appropriate applications of a given polymorph. To understand the thermal stability of new high explosive 4,4′,5,5′-tetranitro-1H,1′H- [2,2′-biimidazole]-1,1′-diamine (DATNBI), we systematically investigated its polymorphic transition (PT) under thermal stimulation and discovered a novel stable γ form of DATNBI. The results showed that the solid-solid PT path was β → α → γ . In this study, the three polymorphs of DATNBI were prepared through solvent recrystallization, and their PT processes in solution were explored. Crystal structure analysis of γ -DATNBI suggested that its special cross-cross grid crystal packing may be the main reason for its stable existence at room temperature and its lack of PT process before chemical decomposition, which starts at 240 °C. To further explore the PT process of DATNBI, the solid phase transition mechanism of DATNBI was analyzed using non-isothermal kinetics. The results demonstrated that the two high-temperature PT processes— β → α and α → γ —were not single-step reactions but complex multi-step reactions. The PT activation energy of the β → α process was slightly higher than that of the α → γ process. In addition, the influences of different polymorphs on the performance of DATNBI were explored. The results revealed that safety and detonation performance should decrease as a result of the incorporation of γ -DATNBI. This study contributes to understanding the PT behavior and the crystal structure evolutionary mechanism of DATNBI. This study provides practical support for formula design, process condition selection, and thermal stability evaluation of DATNBI explosives.
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INORGANIC CHEMISTRY
·
2020
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IF 4.825
Ji Wu,Ke Cao,Cai-Yan Zhang,Tao-Tao Xu,Xin-Yu Wen,Bo Li,Junxiao Yang
A palladium catalyzed selective B(3)–H activation/oxidative dehydrogenative coupling for the synthesis of bis(o-carborane)s connected with B(3)–B(3′) and B(3)–B(6′) bonds has been developed for the first time. A plausible mechanism involving stepwise activation of B(3)–H and B(3′/6′)–H bonds by PdII and PdIV was proposed. This work is the first example and the most efficient protocol for synthesis of bis(o-carborane)s connected with B(3)–B(3′) and B(3)–B(6′) bonds, which has important reference for design, synthesis, and application of bis(o-carborane)s in related fields.
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JOURNAL OF ORGANIC CHEMISTRY
·
2025
·
IF 3.6
Jiapeng Sun,Hanxiao Luo,Junyong Wang,Hongliang Li,Raorao Zheng,Dingru Qiao,Jiaji Zhao,Yue Yu,Hua Cao
A simple and practical method has been developed for the carbonylative esterification of imidazo[1,2-a]pyridines via C(sp2)–H bond functionalization using alkyl alcohols under mild reaction conditions. The carbonyl fragment is sourced from radical-mediated C–C cleavage of the alcohols, providing a green, safe, and economic alternative to traditional carbonyl sources like carbon monoxide. Through this strategy, a number of imidazo[1,2-a]pyridine-3-carboxylates were obtained from simple substrates by a single step.
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PubMed
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