Nature Synthesis
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2026
·
IF 22.6
Zhang Hao,Liu Ziming,Li Di,Wu Chenxin,Hua Lei,Li Haiyang,Yi Yanhui,Huang Rui,Yu Liang,Deng Dehui
Direct co-conversion of earth-abundant N 2 and CH 4 to high-value C–N–O compounds is a promising synthetic method but remains challenging, as the activation of N 2 and CH 4 typically requires high-energy conditions that can cause product decomposition. Here we report a plasma-cascade process for synthesizing cyclohexanone cyanohydrin (Cy(OH)CN) via direct coupling of N 2 and CH 4 plasma with cyclohexanone. This catalyst-free process achieves a Cy(OH)CN formation rate of 0.60 mmol h −1 with a high selectivity of 95.8% towards the cyclohexanone-derived products under mild conditions, concurrently generating ammonia as a valuable coproduct. Comprehensive mechanistic studies reveal that plasma-generated ·CH x and hydrogen radicals enable direct α-carbonyl functionalization of cyclohexanone to α-CH x cyclohexanol intermediates, which then coupled mainly with excited-state N 2 and are further activated by hydrogen radicals to generate Cy(OH)CN. This plasma-cascade strategy decouples the activation of inert molecules from the formation of relatively unstable C–N–O compounds, enabling selective cyanohydrin synthesis that avoids using high-cost NH 3 and toxic HCN. The alternative text for this image may have been generated using AI.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
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IF 9.1
Ating Li,Shuangjiang Li,Bo Wang,Tan Li,Wenbo Zhao,Honghong Liu,Zhiyong Xu
Constructing porous carbon adsorbents with SF 6 -matched ultramicropores is an effective route for recovering SF 6 from nitrogen-rich gas streams. Herein, hemin was introduced into ZIF-8 precursors to regulate pyrolysis-induced pore evolution and produce Fe,N-containing porous carbons without corrosive KOH activation. The optimized Fe,N-C-1000 displayed a large BET surface area of 1772.60 m 2 ·g −1 along with abundant ultramicropores mainly distributed at 0.5–0.65 nm, providing suitable confined spaces for adsorption of SF 6 . The Fe,N-C-1000 delivered an SF 6 adsorption capacity of 4.58 mmol·g −1 and an IAST selectivity of 222 at 298 K and 1.0 bar. Fixed-bed breakthrough tests verified the preferential retention of SF 6 over N 2 , as well as good regenerability and cycling stability. Structure-performance analysis suggests that the improved separation performance is mainly governed by hemin-directed ultramicropore formation, while the Fe/N-containing surface environment contributes additionally to SF 6 affinity. DFT calculations further support stronger SF 6 interaction with the Fe,N-C model than with the undoped carbon model. These results demonstrate that hemin-assisted pyrolysis provides a feasible KOH-free strategy for constructing MOF-derived ultramicroporous carbons for the capture and recovery of SF 6 .
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Journal of Materials Chemistry A
·
2026
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IF 9.2
Yueling Chen,Shibin Zheng,Xingci Huang,Zhangtong Zhang,Guocheng Huang,Qiaoshan Chen,Ling Wu,Jinhong Bi
Covalent organic frameworks (COFs) have emerged as promising candidates for photocatalytic CO2 reduction. While the introduction of single metal atoms can enhance activity, most reported COF-single atoms catalysts adopt near-planar coordination environments that confine carrier migration largely within individual layers, imposing high interlayer transfer barriers and sluggish kinetics and consequently hindered overall performance. This work constructed a single-atom Ag-modified covalent organic framework (Ag-COF) by confining isolated Ag atoms within a spherical TD-COF scaffold, thereby wiring adjacent layers into efficient interlayer charge-transfer channels for gas-solid CO2 photoreduction. Under visible light and without sacrificial agents, Ag0.15-COF delivered a CO formation rate of 184.05 μmol·L-1 with near-unity CO selectivity, representing a tenfold improvement over pristine TD-COF. Structural and photoelectronic analyses identified the N-Ag-N bridging motifs that lowered the interlayer electron-transfer barrier, accelerated carrier separation/migration, and tuned the local electronic structure of active sites. In situ spectroscopy combined with thermodynamic calculations further revealed that the strengthened interlayer charge flow enhanced CO2 adsorption/activation and markedly reduced the barrier for forming the key *COOH intermediate. This study elucidates, at the atomic scale, how interlayer charge transfer governs the activity and selectivity, and provides a design blueprint for highly efficient single-atom-modified COF photocatalysts.
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Catalysts
·
2026
·Vol. 16
·期 8
·689
·
IF 4.5
Zhongqiang Bao,Yiwei Zhang,Zhenhua Ji,Zhenguo Li,Peng Zhang,Ding Luo,Zhanming Chen,Han Gao,Lei Zhu,Hao Chen
Supported Pt catalysts are highly active for the selective catalytic oxidation of ammonia (NH3-SCO), but their practical use is limited by poor N2selectivity and insufficient hydrothermal durability under high-temperature exhaust conditions. Herein, we report a composition-regulated high-entropy oxide interface strategy to stabilize Pt–Cu dual sites and steer NH3oxidation toward selective N2formation. A series of fluorite-type Ce-based high-entropy oxides, including CeZrLaPrYOx, CeSmLaPrYOx, and CeSnLaPrYOx, were constructed as thermally robust supports for Pt and Cu loading. Among them, PtCu/HEO-Zr calcined at 1000 °C exhibits the best NH3-SCO performance, achieving 90% NH3conversion at 260 °C while maintaining N2selectivity above 80% over a broad temperature window of 100–300 °C under a high weight hourly space velocity of 100,000 mL·g−1·h−1. More importantly, after harsh hydrothermal aging at 800 °C with 10 vol% H2O for 12 h, the catalyst shows negligible activity loss and nearly unchanged N2selectivity, demonstrating exceptional structural and catalytic robustness. Structural and surface analyses reveal that Zr incorporation optimizes the fluorite high-entropy lattice, increases oxygen vacancy concentration, promotes lattice oxygen mobility, strengthens surface acidity, and enriches active Cu2+species, thereby enhancing the interfacial cooperation between NH3activation and oxygen-assisted intermediate conversion. In situ DRIFTS further reveals that PtCu/HEO-Zr favors an Olat-assisted internal selective catalytic reduction pathway, in which adsorbed NH3is activated to -NH2species and subsequently reacts with lattice oxygen-derived intermediates to form N2O22−-like species that decompose into N2and H2O. Meanwhile, the formation of nonselective NOxand N2O products is suppressed. This work highlights high-entropy oxide-supported Pt–Cu interfaces as a promising platform for designing hydrothermally durable and N2-selective NH3-SCO catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Cancan Yang,Yugao Wang,Jiaxin Jing,Linyuyang Shi,Jinping Li,Jiangfeng Yang
Activated carbon (AC) is a commonly used and readily available adsorbent for CH 4 and N 2 adsorption separation, however, it is seriously hindered by the uneven micropore size distribution of AC and inappropriate microporous size. In this work, a commercial AC was modified with CuCl 2 for addressing the limitation and thereby enhancing CH 4 /N 2 adsorption separation performance. According to in-situ X-ray diffraction analysis, Cu species were volatilized in the form of CuCl functioning as a dynamic porogen during thermal treatment. The process homogenized the initially irregular and broad pore size distribution of the original AC, which accounted for enhancing CH 4 /N 2 adsorption separation selectivity from 4.44 to 7.53. This investigation provides a powerful and potential modification approach for enhancing CH 4 /N 2 adsorption separation performance of the commercial AC.
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JOURNAL OF FOOD SCIENCE
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2025
·Vol. 90
·期 6
·e70310
·
IF 3.4
Arooj Rehman Sheikh,Miral Javed,Hao Zhang,Qiaojun Jia,Zisheng Luo
Camellia oleifera shells, waste material obtained after oil extraction, contain a significant number of terpenes. This study introduces a novel, eco-friendly, and sustainable method to combine N 2 -NBs with limonene and ultrasound to enhance terpene extraction from food waste. N 2 -NBs suspension stabilized by Tween 80, resulting in 255 nm size with reduced surface tension. Raman spectroscopy indicates strong hydrogen bonding at 1646 cm⁻¹, suggesting that the enhanced release of compounds and micelle formation improved the solubility of terpenes. Meanwhile, SEM demonstrated that the collapse of N 2 -NBs effectively disrupted cell walls. Together, these mechanisms significantly enhanced terpene compounds' release, solubility, and overall yield. Combining Tween 80 and N 2 -NBs with ultrasound achieved a terpene yield of 42.88 ± 1.87 mg/g DW, significantly higher than the 10.96 ± 2.87 mg/g DW from ethanol extraction. These findings highlight the novel eco-friendly approach to effectively extract terpenes, which can be useful for industrial applications. Practical applications The novel, eco-friendly extraction method can be used to reuse food waste. High-yielding extraction method can be used to extract pharmaceutical compounds. Extracted terpenes can be used for various food industry applications.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
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2024
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IF 8.1
Shaopeng Yu,Ya Liu,Jiangyong Cao,Shibao Wen,ZhenXiu Zhang
The development of efficient and environmentally friendly rubber foams is crucial for reducing fire hazards and protecting lives and property. Herein, this study developed a green microcellular foaming method for lightweight and high-strength chloroprene rubber (CR) flame-retardant foams. A strategy that actively releases H 2 O and rapidly forms carbon to stop flames is proposed by low-toxicity smoke suppression aluminum hydroxide (ATH) and readily carburizable Zinc borate (ZB) as flame retardants. Based on the quantitative information of the cellular structure, the effects of ATH and ZB on the foaming behaviors of CR foams were investigated. Thanks to its excellent compounding effect, a significant increase in the limiting oxygen index up to 36.5 % is achieved with a density of 0.263 g/cm 3 . It also demonstrated excellent smoke suppression with a low total smoke production of 0.19 m 2 , a reduction of 96.6 % compared to pure CR foam. In addition, the incorporation of ATH and ZB effectively improves its mechanical properties and thermal conductivity. This study provides a new path manufacture CR foam with excellent overall performance, which effectively improve the overall safety and energy efficiency of the building.
研究领域:
材料科学
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高分子化学
·
防火材料
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Mao Ye,Hexiang Huang,Lei Tian,Xiujing Zhang,Ziyao Wang,Chenxu Zhang,Zhihua Qiao
Separation of CH 4 and N 2 from natural gas is essential to increase energy efficiency and reduce environmental impact. In this work, we prepared novel mixed matrix membranes (MMMs) for CH 4 /N 2 separation using ion-exchange-modified molecular sieves as fillers and metal–organic framework (MOF) glass as substrates. The modification of molecular sieves enhanced the gas separation capability of the MMMs. And the MOF glass as a matrix has good compatibility with the filler. The membrane achieved a CH 4 permeance of up to 271.4 GPU and a CH 4 /N 2 selectivity of 7.35. The membrane was able to maintain stable separation performance under certain pressures and over a long testing period. The design of this study provides an innovative approach to advancing natural gas applications.
研究领域:
化学工程
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材料科学
·
膜技术
·
分离过程
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环境科学
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JOURNAL OF MEMBRANE SCIENCE
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2017
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IF 6.035
Hui Li,Xiaoxu Ding,Yatao Zhang,Jindun Liu
The inherent defects of porous graphene (PG) formed during reduction etching process could serve as nanopores , making PG emerge a potential application for the preparation of micrometre-sized separation membranes . Here, we introduced PG as inorganic nanofiller to fabricate thin film nanocomposite (TFN) membranes for CO 2 capture via interfacial polymerization technique. The PG selective nanolayers not only possessed a good adhesion with polymers but also benefited from hydrogen bonding actions, simultaneously, thus ensuring the formation of high-efficiency molecular sieving passageway in the separation layer of membranes. Furthermore, the thin PG nanosheets were verified to have an significantly affect for permeability and selectivity of membranes (PG, 0.05 wt%, 1 bar), with exhibiting about 21% and 20.8% enhancement of the CO 2 permeance and the CO 2 /N 2 selectively compared to that of the membrane without PG separately. Simultaneously, the membrane also showed higher stability and the porous surface morphology of PG shortened greatly the gas transfer path. The approach offers a potential promising to exploit the ultra-thin film composite membrane for efficient gas separation.
研究领域:
材料科学
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环境科学
·
化学工程
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ACS Sustainable Chemistry & Engineering
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2018
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IF 6.14
Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Yuanchao Pei,Yongkui Chen,Jianji Wang
Emulsion inversion has great potential in applications such as materials science, chemical reactions, and drug delivery. Therefore, developing a simple and green approach to control emulsion inversion is highly desirable. Herein an octyl- and bis(2-hydroxyethyl)-3-amino-bifunctionalized silica microsphere (SM-O-BIS) is designed, prepared, and used to fabricate a Pickering emulsion. It is found for the first time that this Pickering emulsion can be easily and reversibly inverted from water-in-oil (w/o) to oil-in-water (o/w) by alternate bubbling of CO2 and N2 at room temperature and atmospheric pressure. The molar ratio of trimethoxyoctylsilane to bis(2-hydroxyethyl)-3-aminopropyltriethoxysilane on the surface of silica is important for the emulsion inversion. This unique inversion can be recycled multiple times without any deterioration. By utilizing the emulsion inversion strategy, encapsulation and release of curcumin molecules have been actualized on demand. The possible mechanism of emulsion inversion is also investigated by measuring zeta potential, water contact angle, 13C NMR spectroscopy, and FT-IR spectroscopy. It is shown that a significant and reversible change in hydrophilicity/hydrophobicity of SM-O-BIS is the driving force for such a CO2/N2-triggered inversion.
研究领域:
材料科学
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化学工程
·
药物递送
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
De Ao,Fujiang Geng,Mao Ye,Shuangjie Yuan,Fanpeng Meng,Jinxiao Bao,Zibo Yang,Zhihua Qiao
The development of high-performance membranes for CO 2 /N 2 separation remains challenging due to the trade-off between permeability and selectivity. A novel strategy has been developed to fabricate K,Na-A zeolite/ZIF-62 crystal-glass composite membranes through a melt-quenching process. The high viscosity of molten ZIF-62 enables the uniform distribution of zeolite particles, preventing their aggregation and sedimentation. The synergistic effect between the highly porous K,Na-A zeolite and the continuous ZIF-62 glass matrix leads to enhanced membrane porosity and efficient gas transport channels. Benefiting from the molecular sieving effect of K,Na-A zeolite and the excellent interfacial compatibility of ZIF-62 glass matrix, the composite membranes demonstrate superior gas separation capability. Systematic investigation revealed that the optimized a g (ZIF-62) 0.7 /(K,Na-A) 0.3 membrane exhibited remarkable CO 2 separation performance with a CO 2 permeability of 58,824 barrer and a CO 2 /N 2 selectivity of 43.1, surpassing the 2019 upper bound. This facile and scalable strategy opens up new opportunities for developing high-performance composite membranes for practical gas separation applications.
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Small
·
2023
·
IF 13.3
Heng Guo,Peng Yang,Yuantao Yang,Haoran Wu,Fengying Zhang,Zhen-Feng Huang,Guidong Yang,Ying Zhou
Ambient electrocatalytic nitrogen (N 2 ) reduction has gained significant recognition as a potential substitute for producing ammonia (NH 3 ). However, N 2 adsorption and *NN protonation for N 2 activation reaction with the competing hydrogen evolution reaction remain a daunting challenge. Herein, a defect-rich TiO 2 nanosheet electrocatalyst with PdCu alloy nanoparticles (PdCu/TiO 2−x ) is designed to elucidate the reactivity and selectivity trends of N 2 cleavage path for N 2 -to-NH 3 catalytic conversion. The introduction of oxygen vacancy (OV) not only acts as active sites but also effectively promotes the electron transfer from Pd-Cu sites to high-concentration Ti 3+ sites, and thus lends to the N 2 activation via electron donation of PdCu. OVs-mediated control effectively lowers the reaction barrier of *N 2 H and *H adsorption and facilitates the first hydrogenation process of N 2 activation. Consequently, PdCu/TiO 2−x catalyst attains a high rate of NH 3 evolution, reaching 5.0 mmol g cat. −1 h −1 . This work paves a pathway of defect-engineering metal-supported electrocatalysts for high-efficient ammonia electrosynthesis.
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