Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Wang Peng,Zhao Danyang,Zhang Peng,Hui Xiaobin,Zhang Zhiwei,Wang Rutao,Wang Chengxiang,Ge Xiaoli,Liu Xiaojing,Li Yuguang C.,Yin Longwei
The metallic phase MoS 2 (1T-MoS 2 ) supported metal-nanocatalyst is an appealing material system for accelerating the redox kinetics of non-aqueous Li | |O 2 batteries. However, the drawbacks associated with the surface orbital steric effect and the internal electron coupling results in a detrimental effect for the stability of 1T-MoS 2 , especially for the interface charge transfer. This makes it difficult to incorporate guest metal nanoparticles without compromising the 1 T phase support. To circumvent these issues, here we propose a p-block element (In-O) doping strategy to stabilize the 1 T phase MoS 2 by moderating the surface orbital steric effect and strengthening the internal chemical bonding, and thus for the epitaxial Ru nanocatalyst graft on the stabilized 1T-MoS 2 for Li | |O 2 batteries. The experimental and theoretical analyzes indicate that the In-O-MoS 2 @Ru enhances the O 2 dissociation and facilitates the adsorption of LiO 2 intermediates. This effect promotes the growth of weakly crystalline Li 2 O 2 films during oxygen reduction reaction, which can be more easily decomposed during the oxygen evolution reaction, thereby enhancing the bifunctional-catalytic kinetics. When employed at the positive electrode for non-aqueous Li | |O 2 batteries, In-O-MoS 2 @Ru shows an overpotential of 0.37 V and a cycling life of 284 cycles at 200 mA g −1 with a final discharge specific capacity of 1000 mAh g −1 at 25 °C.
研究领域:
材料科学
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电化学
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储能技术
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纳米技术
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
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2025
·
IF 6.7
Lei Zou,Lu Wei,Yubei Liu,Mingjie Huang,Xiangling Zhang,Wenjiao Sang,Shuting Li,Chen Wang,Wei Xiang
The pervasive threat of toxic and stable heavy metal-organic complexes to aquatic ecosystems necessitates efficient decomplexation strategies. In this study, we developed a magnetic field (MF)-enhanced nano zero-valent iron (nZVI) system that activated O 2 for the removal of Cu(II) and chemical oxygen demand (COD) from Cu-complexed wastewater (EDTA-Cu, citrate-Cu, tartrate-Cu). The introduction of MF significantly enhanced Cu-complex destruction and Cu 2+ immobilization, while reducing toxicity and improving biodegradability. Mechanistic studies revealed that nZVI would displace Cu from complexes, reducing free Cu 2+ to Cu 0 on its surface. The resultant Cu 0 , in synergy with Fe 2+ , activated O 2 to generate reactive oxygen species (ROS), which cleaved metal-organic bonds and oxidized organic ligands. MF amplified this process by enhancing paramagnetic O 2 accumulation at nZVI/Cu 0 sites, accelerating ROS production via the O 2 ⟶O 2 •− ⟶H 2 O 2 ⟶•OH pathway, thereby boosting Cu-organic decomplexation and COD removal. Catalyst characterization further revealed that MF promoted Cu 0 dispersion on nZVI, preventing cluster formation and optimizing electron utilization for O 2 activation. As demonstrated by our energy-cost efficiency analysis, the MF/nZVI/O 2 process achieved 1.375–1.785 g Cu /kWh for Cu-organic wastewater treatment, significantly outperforming many previously reported processes. This study introduces a novel MF-assisted nZVI system for efficient treatment of Cu-complexes, offering a promising cost-effective and sustainable solution for practical application.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
高影响因子
Scientific Reports
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2025
·Vol. 15
·期 1
·1-14
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IF 3.9
Liu Liming,Lian Hongxia,Deng Heming,Zhang Weixin
Challenges associated with the cathode material of Lithium–oxygen (Li–O 2 ) battery, particularly the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction, as well as the accumulation of discharge product Li 2 O 2 , have hindered its further advancement. Here, an in-situ synthesis strategy was adopted to load a bimetallic Ni–Co metal–organic framework (Ni/Co-MOF) onto MXene (Ti 3 C 2 ) layers. Subsequently, a free-standing and flexible Ni/Co-MOF@Ti 3 C 2 hybrid membrane is prepared via a layer-by-layer self-assembly method, specifically designed for efficient ORR and as a cathode for Li–O 2 batteries. The Ni/Co-MOF@Ti 3 C 2 hybrid membrane integrates the high conductivity, unique two-dimensional layered structure, and excellent mechanical properties of Ti 3 C 2 with the bimetallic active sites of Ni/Co-MOF, exhibiting remarkable ORR catalytic activity in an O 2 -saturated 1 M LiTFSI electrolyte. The structural characteristics of the hybrid membrane provide smoother expansion pathways for Li + and O 2 , effectively promoting the deposition and decomposition of Li 2 O 2 . This not only enhances the electrochemical performance of the Li–O 2 battery but also overcomes the inherent limitations of traditional slurry-based cathode preparation methods. Experimental results demonstrate that Li–O 2 batteries utilizing the Ni/Co-MOF@Ti 3 C 2 hybrid membrane as the cathode achieve an ultra-high capacity of 36,125 mAh/g at a current density of 1000 mA/g, while exhibiting excellent cycle stability (271 cycles with a limited capacity of 1000 mAh/g at 1000 mA/g) and outstanding rate performance. The hybrid membrane’s capacity and cycle performance can be further optimized by controlling its thickness. These promising results offer novel insights into the innovative design of air cathodes for metal–air batteries, and the proposed method provides a new route for the manufacture of high-performance battery cathodes.
研究领域:
材料科学
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电化学
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能源存储与转换
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2020
·Vol. 9
·期 5
·1593-1603
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IF 7.059
Guoming Gao,Ximeng Wang,Qifeng Chen,Caibo Xie,Jie Zheng,Huailin Fan,Lulu Ma,Ruifang Guan,Yanfen Fang,Xun Hu
Surface fluorinated TiO2 has received extensive attention in recent years due to the improved photocatalytic reactivity compared with that of pure TiO2. However, the synergy of surface fluorine (FS) and oxygen vacancy (VO) is not clear and needs further study. Here we systematically studied the effect of FS, VO and acidic sites of TiO2 nanosheets on the selective photocatalytic oxidation of benzylamine to imine. The photocatalytic activity first increased and then decreased as the content of FS decreased and VO increased. The photocatalytic activity reached a summit with the imine yield of 92.1% over TiO2-B-6 h, which is mainly due to the synergy between FS and adjacent VO, forming the frustrated Lewis pair that boosts the activation of O2. The varied contents of FS and VO not only cause an evident change in the amount of acidic sites, but also affect the band structure and separation efficiency of charge carriers. The experimental and calculation results demonstrate that the coexistence of FS and VO boosted the separation efficiency, density and mobility of photogenerated charge carriers, resulting in the improved photocatalytic activity. The improved photocatalytic activity can be attributed to the combined effects of FS, VO and acidic sites. This work provides a strategy for the explicit regulation of surface species on TiO2 nanosheets for improved photocatalytic activity.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Catalysts
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2025
·Vol. 15
·期 7
·694
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IF 4
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
The development of non-noble metal catalysts for gas-phase propylene epoxidation with H2/O2remains challenging due to their inadequate activity and stability. Herein, we report a Cs+-modified Ni/TS-1 catalyst (9%Ni-Cs/TS-1), which exhibits unprecedented catalytic performance, giving a state-of-the-art PO formation rate of 382.9 gPO·kgcat−1·h−1with 87.8% selectivity at 200 °C. The catalyst stability was sustainable for 150 h, far surpassing reported Ni-based catalysts. Ni/TS-1 exhibited low catalytic activity. However, the Cs modification significantly enhanced the performance of Ni/TS-1. Furthermore, the intrinsic reason for the enhanced performance was elucidated by multiple techniques such as XPS, N2physisorption, TEM,29Si NMR, NH3-TPD-MS, UV–vis, and so on. The findings indicated that the incorporation of Cs+markedly boosted the reduction of Ni, enhanced Ni0formation, strengthened Ni-Ti interactions, reduced acid sites to inhibit PO isomerization, improved the dispersion of Ni nanoparticles, reduced particle size, and improved the hydrophobicity of Ni/TS-1 to facilitate propylene adsorption/PO desorption. The 9%Ni-Cs/TS-1 catalyst demonstrated exceptional performance characterized by a low cost, high activity, and long-term stability, offering a viable alternative to Au-based systems.
研究领域:
催化化学
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化学工程
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材料科学
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多相催化
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绿色化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2025
·
IF 9.5
Guangqi Zhang,Congcong Dang,Yiping Liu,Rouyan Guo,Lingti Kong,Liancheng Zhao,liming Gao
Li-O2 batteries have emerged as promising contenders for advanced energy storage systems, leveraging their exceptionally high theoretical energy density. Nevertheless, their practical deployment is substantially hindered by rapid capacity degradation and restricted operational durability, primarily attributed to sluggish oxygen reaction kinetics. Here, to modulate kinetic barriers, we propose an approach synergizing structural and electronic advantages by integrating heterointerface engineering and hierarchical nano structuring. A hollow nanobox MoSe2@CuS core-shell heterostructure is developed as a bifunctional oxygen electrode. Such heterostructure could induce a built-in electric field to modulate charge transfer dynamics and the hollow architecture could optimize triple-phase interfacial reactions. Leveraging the synergistic attributes of its components, the MoSe2@CuS-based Li-O2 battery achieves an excellent specific capacity of 16,000 mAh g-1 at 100 mA g-1. Moreover, it demonstrates remarkable cycling durability, sustaining high performance for over 190 cycles at 200 mA g-1 with a restricted capacity of 600 mAh g-1. Density functional theory (DFT) calculations further illustrate the lowered energy kinetic barrier for Li2O2 formation/decomposition induced by MoSe2@CuS core-shell heterostructure. This work pioneers a universal heterointerface engineering strategy through rational design of hierarchical hollow architectures, providing new insights for developing high-performance Li-O2 battery cathodes.
研究领域:
储能
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纳米材料
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电化学
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电池技术
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材料科学
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理论化学
✓ 已验证
DOI
高影响因子
Materials Today Communications
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2025
·
IF 4.5
Jiaqi Wang,Xiqiang Huang,Xingbao Zhu,Yuanguo Wu,Zining Man,Xiangyu Wen,Weiting Qi,Xing Tang,Zhe Lü
Despite their potential to enhance safety and design flexibility in next-generation lithium batteries, particularly lithium-oxygen (Li-O 2 ) systems, solid polymer electrolytes (SPEs) face persistent challenges of insufficient ionic conductivity and high interfacial resistance. To address these limitations, we developed a novel PEGDA-based quasi-solid-state electrolytes (QSEs) through in situ polymerization, strategically incorporating three functional additives: cellulose acetate (CA), N-methyl-2-pyrrolidone (NMP), and fluoroethylene carbonate (FEC). The electrolyte design leverages multiple synergistic mechanisms: hydrogen bonding between CA and NMP optimizes microstructural organization for efficient Li⁺ transport pathways; carbonyl groups in NMP coordinate with Li⁺ to facilitate LiTFSI dissociation, while oxygen-rich functional groups in CA provide supplementary Li⁺ coordination sites; FEC is introduced to further improve interfacial stability. This molecular engineering approach achieves an impressive room-temperature ionic conductivity of 8.54 × 10 −4 S cm −1 and a high lithium-ion transference number of 0.78. The QSE demonstrated excellent cycling stability (>900 h) in lithium symmetrical batteries and significantly improved the discharge capacity (12243 mAh g −1 ) and long-term cycling performance (590 h) of Li-O 2 batteries. These results highlight the efficacy of our multi-functional additive strategy in overcoming fundamental limitations in solid electrolytes, offering important insights for the rational design of high-performance energy storage systems.
研究领域:
储能
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材料科学
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电化学
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聚合物电解质
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
Chem
·
2019
·
IF 18.205
Rongan Shen,Wenxing Chen,Qing Peng,Siqi Lu,Lirong Zheng,Xing Cao,Yu Wang,Wei Zhu,Juntao Zhang,Zhongbin Zhuang,Chen Chen,Dingsheng Wang,Yadong Li
Summary The electrochemical direct synthesis of hydrogen peroxide (H 2 O 2 ) is significant but still challenging because of the lack of highly selective and active catalysts. Here, we report the synthesis of hollow nanospheres constructed by atomically dispersing platinum in amorphous CuS x support (h-Pt 1 -CuS x ) with a high concentration of single atomic Pt sites (24.8 at%), and this catalyst can consistently reduce O 2 into H 2 O 2 with selectivity of 92%–96% over a wide potential range of 0.05–0.7 V versus RHE in HClO 4 electrolyte. Scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy confirmed the atomically isolated form of Pt with a low valance of +0.75. An electrochemical device that can synthesize H 2 O 2 directly from H 2 and O 2 is fabricated with H 2 O 2 productivity as high as 546 ± 30 mol kg cat − 1 h −1 . The well-defined and high-concentration single atomic Pt sites result in ultrahigh productivity of H 2 O 2 .
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zehui Fan,Zhisen Li,Dan Mo,Jingyang Zhang,Shuyi Yang,Yun Li,Changlong Bi,Chong Peng,E Tao
Modulation of nano electrocatalysts for targeted excitation of different reactive oxygen species (ROS) is a key challenge to achieve environmentally catalyzed efficient pollutant degradation. In this study, multivalent copper catalysts (Cu (0)/Cu (I)/Cu (II)) load on the surface of biochar (CBX) are prepared by the hydrothermal-impregnation method, and the modulation effect of different valences of copper on the pathway of reactive oxygen species (ROS) generation is investigated. X-ray diffraction (XRD) analysis shows the coexistence of three copper valence states. Radical scavenging experiment and DFT calculations indicate that Cu (I) dominates the adsorption and activation of peroxodisulfate (PS) to efficiently generate ·SO 4 - and ·OH. Cu (II) selectively generates 1 O 2 by modulating the dissolve oxygen conversion pathway; whereas Cu (0) acts as an activation center for bound oxygen and significantly promotes ·O 2 - generation. The nano-electrocatalytic system prepared at 600°C (CB6-PS) degraded 98.3% of enrofloxacin (ENR) over a period of time (60 min). Mechanistic studies indicate that the catalytic system realizes the coupling reaction between the radical pathway (·SO 4 - /·OH /·O 2 - ) and the nonradical pathway ( 1 O 2 ) by the synergistic action of multivalent copper, which providing a new theoretical basis and technical strategy for the development of targeted ROS generation function.
研究领域:
环境催化
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材料化学
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污染控制
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纳米催化
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环境功能材料
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高级氧化技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Qiming Song,Zifan Li,Qun Peng,Xinwen Ou,Kun Zhao,Zhimin Dong,Liqun Ye,Chenchen Liu,Yunhai Liu,Jun He,Lai-Hon Chung,Bin Han
Photocatalytic O 2 activation, which produces miscellaneous reactive oxygen species (ROSs) via electron or energy transfer, is crucial for various chemical and biological processes. Unfortunately, controlling the exciton behaviors to flexibly regulate the generation of ROSs has rarely been explored and the underlying regulatory mechanisms remain poorly understood. Here, via linkage orientation engineering of covalent organic frameworks (COFs), we showcase a facile strategy for the flexible regulation between 1 O 2 and H 2 O 2 generation in photocatalytic O 2 activation. Imine-based COFs equipped with donor (D)-N=C-acceptor (A) chain (TFPT COFs) exerts effective H 2 O 2 production via electron transfer, while its structurally isomeric COFs with reversed imine orientation (TAPT COFs) tends to singlet oxygen ( 1 O 2 ) photosynthesis via energy transfer, attaining high efficiency for pollutant removal. Based on the results from ultrafast spectroscopy and theoretical calculations, when the N atom of the imine linkage is close to the electron acceptor, it diminishes the surface potential difference and increases the exciton binding energy; this favors the activation of the spin-triplet state excitons via an energy transfer process. Conversely, a strong built-in electric field is created when this N atom is adjacent to the electron donor, which encourages the dissociation of excitons into carriers and their subsequent separation.
研究领域:
化学
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材料科学
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生物学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 31
·2404319
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IF 27.4
Zongqiang Sun,Xiaodong Lin,Chutao Wang,Yanyan Tan,Wenjie Dou,Ajuan Hu,Jiaqing Cui,Jingmin Fan,Ruming Yuan,Mingsen Zheng,Quanfeng Dong
Lithium–oxygen (Li–O 2 ) batteries, renowned for their high theoretical energy density, have garnered significant interest as prime candidates for future electric device development. However, their actual capacity is often unsatisfactory due to the passivation of active sites by solid-phase discharge products. Optimizing the growth and storage of these products is a crucial step in advancing Li–O 2 batteries. Here, a fluorine-doped bimetallic cobalt-nickel oxide (CoNiO 2– x F x /CC) with an interlaced catalytic surface (ICS) and a corncob-like structure is proposed as an oxygen electrode. Unlike conventional oxide electrodes with a “single adsorption catalytic mechanism,” the ICS of CoNiO 2− x F x /CC offers a “competitive adsorption catalytic mechanism,” where oxygen sites facilitate oxygen conversion while fluorine sites contribute to the growth of Li 2 O 2 . This results in a change in Li 2 O 2 morphology from a surface film to toroidal particles, effectively preventing the burial of active sites. Additionally, the unique open architecture aids in the capture and release of oxygen and the formation of well-contacted Li 2 O 2 /electrode interfaces, which benefits the complete decomposition of Li 2 O 2 products. Consequently, the Li–O 2 battery with a CoNiO 2− x F x /CC cathode demonstrates a high specific capacity of up to 30923 mAh g −1 and a lifespan exceeding 580 cycles, surpassing most reported metal oxide-based cathodes.
研究领域:
材料科学
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电化学
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能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 13
·e202303633
·
IF 1.9
Mingyan Chen,Wentao Wang,Xinkai Feng,Dehua Zhang,Yao Zhang,Yucheng Liu
Graphical This work describes the application of a highly efficient catalyst (NH 2 -UiO-66-Mo) to the catalytic oxidation desulfurization process. NH 2 -UiO-66-Mo can greatly improve the efficiency of oxidative desulfurization The optimum operating conditions of NH 2 -UiO-66-Mo are investigated through experiments, which prove the excellent performance of the catalyst, and the reaction mechanism is further studied through a series of characterizations. A highly efficient oxidative desulfurization composite catalyst NH 2 -Uio-66-Mo has been prepared and applied in the catalytic oxidative desulfurization. It was elucidated that Mo 6+ could increase the oxygen vacancies and active sites on the catalyst and increase the pore size of UiO-66. Meanwhile, the removal rate of dibenzothiophene (DBT) reached 99.2 % after 60 min under optimal conditions and remained above 90 % after 5 cycles, showing the composite catalyst's remarkable catalytic performance and satisfactory reusability NH 2 -UiO-66-Mo. In addition, kinetic studies revealed that the desulfurization process can present a pseudo-first-order kinetic process. The apparent activation energy was 10.6 kJ/mol. Finally, in combination with oxides, possible oxidation pathways were identified.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）