FUEL
·
2020
·
IF 5.578
Jing-Pei Cao,Tao Xie,Xiao-Yan Zhao,Chen Zhu,Wei Jiang,Ming Zhao,Yun-Peng Zhao,Xian-Yong Wei
Selective hydrogenolysis, the aromatic ether C-O bonds under mild conditions, is crucial for the valorization of lignin. In this context, the effects of H 2 and solvent on the hydrogenolysis of lignin model compounds over Ru catalysts were explored. With H 2 as hydrogen donor, the Ru/AC exhibited the highest activity for converting lignin model compounds into monomeric compounds, whereas H 2 led to low selectivity of aromatics. However, isopropanol was the good H-donor solvent, which could provide a large amount of active hydrogen to promote the cleavage of C-O bonds. Additionally, the yield of aromatics in isopropanol was higher than that under H 2 atmosphere. It could be ascribed to the fact that isopropanol is the protic solvent which displays Lewis basicity, and is a good H-bond donor and a good H-bond acceptor. The higher electron-releasing inductive effect of isopropanol made it easier to provide active hydrogen. Based on the experiments, the mechanism of benzyl phenyl ether hydrogenolysis in H 2 and isopropanol system was presented.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Xiaoyue Wan,Qi Zhang,Mingming Zhu,Yi Zhao,Yongmei Liu,Chunmei Zhou,Yanhui Yang,Yong Cao
Site-selective deoxygenation of hydroxyl groups represents essential processes to access valuable functionalized bio-based compounds with industrial potential. One of the challenging tasks in this context is to convert biodiesel-derived glycerol in the presence of abundant water directly to 1,3-propanediol (1,3-PDO), a key component of the emerging polymer industry. Herein, a monometallic iridium supported on H-ZSM-5 in the absence of Re oxophilic metal oxides was prepared via grinding-assisted impregnation procedures and attempted as an effective and recyclable catalyst for the aqueous-phase selective hydrogenolysis of glycerol toward 1,3-PDO in the absence of acid additives. The results revealed the necessity to control the Ir domain dispersions, Ir 0 /Ir 3+ ratio and the amounts of overall acid/Brönsted acid sites. Activity depended linearly on the amount of overall and Brönsted acid sites, and 1,3-PDO selectivity increased in the presence of Ir-induced Brönsted acid sites, denoted as Ir-O(H)-H-ZSM-5. We speculate that Ir-O(H)-H-ZSM-5 are generated by the interfacial synergistic interaction between IrO x and H-ZSM-5 through hydrogen spillover and reverse hydrogen spillover according to the reported literatures. The reaction mechanism to elucidate the role of Ir-O(H)-H-ZSM-5 sites in glycerol hydrogenolysis was also postulated based on extensive characterization and catalytic reaction results.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Huanzhao Liu,Pengxin Li,Yifan Wang,Huijie Wang,Yi Fang,Zhonglu Guo,Yang Huang,Jing Lin,Long Hu,Chengchun Tang,Zhenya Liu
Toxic dyes in wastewater will become a significant hazard to human health if they are not treated effectively. Therefore, it is significant to separate and remove dyes from the aqueous solution. C and O co-doped BN (BCNO) with high adsorption capacity and outstanding cycle efficiency is a simple and efficient adsorbent for the cationic dye malachite green (MG). Glucose is characterized as an eco-friendly and cheap source of C and O. Benefited by the high specific surface area (1515.6 m 2 /g), the maximum adsorption capacity of MG is 1511.1 mg/g. Besides, the curves of adsorption fitting correspond to the Langmuir model and the pseudo-second-order model, respectively. Moreover, after 5 cycles, the adsorption efficiency reached 78% of the first time and the adsorption capacity remained above 780 mg/g. Furthermore, in the selectivity adsorption study, the cationic dyes (MG, neutral red (NR), methylene blue (MB)) can be removed more effectively in the binary dye system of MG-methyl orange (MO), NR-MO, MB-MO, MG-Orange II (OR), MB-OR, or NR-OR. BCNO-2 has a promising application in the removal of cationic dyes from complex dye wastewaters.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lin Ai,Yanping Chen,Fang Lu,Jiaxu Liu,Xiao-Feng Wu,Shengjun Huang
The fundamental challenge in the gas-phase selective hydrogenation of α,β-unsaturated aldehydes to α,β-unsaturated alcohols lies in the construction of microscopic environment for the preferential hydrogenation of C = O bond along with the preservation of C = C bond under the reductive atmosphere. Herein, we proposed a structure-matching strategy for the catalyst design, in which In component in metallic form and oxide form are interplayed with metallic Ni and Al 2 O 3 support, respectively. The fabrication of In-Ni intermetallic compound stokes up the desirable electropositive-electronegative environment (In δ+ -Ni δ- ) for the adsorption of polar carbonyl group. The In species in the In-oxo form are engaged in the network of Al 2 O 3 support in the formation of In-O-Al-O entities, which stabilizes the heterolytically dissociated H species to match the preferential saturation of polar C = O bond. Therefore, the resulting In-Ni-Al 2 O 3 catalyst achieves a selectivity of 77.2 % to methallyl alcohol with a conversion of 53.8 % in the gas-phase hydrogenation process, which present a striking contrast to the outcomes upon the counterpart Ni-Al 2 O 3 (non-selectivity to methallyl alcohol). Such structure-matching strategy enriches the fundamental understandings and basis for the rational design of catalysts for the selective hydrogenation of unsaturated aldehydes.
研究领域:
催化
·
化学工程
·
材料科学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Yang Hu,Xiaoyue Lu,Mingche Huang,Erhong Song,Bowen Chen,Feiyan Cai,Yuefan Xu,Yinjie Ruan,Chaobin Zeng,Ling Lin,Yan Gu,Yusheng Ding,Dewei Ni,Shaoming Dong
The initial oxidation stage of high-entropy carbides (HECs) is a decisive yet poorly understood “black box” that governs their ultimate performance for ultra-high-temperature applications. Here, we unveil a powerful strategy—predesigning carbon vacancies—to fundamentally enhance HECs oxidation resistance. By integrating in situ x-ray diffraction (XRD) and in situ transmission electron microscopy coupled with electron energy loss spectroscopy (TEM-EELS), we provide the first direct, atomic-scale visualization of oxygen atoms preferentially occupying these predesigned vacancies during the incipient oxidation stage, leading to the dynamic formation of a metastable metal–carbon–oxygen (M–C–O) interfacial layer. Our combined experimental and theoretical analyses reveal a dual enhancement mechanism: kinetically, M–C–O suppresses both oxygen adsorption on the (111) surface and its subsequent inward diffusion; thermodynamically, they stabilize the HEC lattice at elevated temperatures, thereby increasing the energy barrier for M─C bond cleavage. This work not only deciphers the atomistic origin of enhanced oxidation resistance but also establishes a simple, general, and efficient design principle for next-generation ultra-high-temperature ceramics.
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DOI
高影响因子
ENERGY & FUELS
·
2026
·Vol. 40
·期 30
·16496-16503
·
IF 6
Zhou Wei,Wu Zhiqian,Li Yanjun,Xu Bing,Wang Xiaoqi,Yang Feifei,Ni Zhonghai
The precise function of metal sites at the bifunctional
metal–oxide
interface in catalytic hydrodeoxygenation (HDO) of biomass-derived
oxygenates remains a subject of debate: do they serve merely as hydrogen
dissociation centers, or do they also directly participate in activating
the oxygenate substrate? To elucidate this, we fabricated two model
Ni/TiO 2 catalysts with distinct surface Ni geometries by
leveraging the crystal phase-dependent strong metal-support interaction.
Ni/r-TiO 2 features exposed surface Ni ensembles, while
Ni/a-TiO 2 presents predominantly isolated Ni sites due
to partial encapsulation by a TiO x overlayer.
Their HDO performance was evaluated using a suite of model compounds,
including m -cresol, anisole, benzyl alcohol, and
furfuryl alcohol, representing key C–O bond types in bio-oils.
The results demonstrate that Ni/r-TiO 2 exhibits broad activity
for all substrates, whereas Ni/a-TiO 2 selectively cleaves
only C–O bonds connected to sp 3 -hybridized carbon
atoms. This fundamental difference originates from the bond dissociation
energy. The cleavage of high-energy C Aromatic –O
bonds necessitates a synergistic activation mode at the Ni ensemble-oxygen
vacancy interface, which, while effective, concomitantly promotes
undesirable ring-related side reactions such as C–C hydrogenolysis,
thereby compromising deoxygenation selectivity. Conversely, lower-energy
C sp 3 –O bonds can be directly activated
on oxygen vacancies assisted by spillover hydrogen from the isolated
Ni sites, enabling precise and selective deoxygenation. This study
clarifies the structure-dependent role of interfacial metal geometry
and provides a mechanistic guideline for the rational design of selective
HDO catalysts tailored to specific feedstock platforms.
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DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2017
·
IF 1.179
Lala Rukh Sidra,Nafeesa Mushtaq,Guofei Chen,Xingzhong Fang
A series of poly(N-arylene benzimidazole ether imide) copolymers PEIBIs were prepared from 1H,3′H-5,5′-bis-benzimidazole, bisphenol-A and 4,4′-bis(4-fluorophthalimido)diphenyl ether by nucleophilic displacement polymerization. The resulting copolymers PEIBI(10–90) demonstrated moderate to good solubility in polar aprotic solvents and high glass transition temperatures (Tgs) of 228–336°C, good thermal stability with 10% weight loss temperatures in the range of 503–548°C. All copolymer films showed good mechanical properties with tensile strengths of 101–130 MPa, tensile moduli of 3.3–4.0 GPa, elongations at break of 5–7%, and also presented low water uptake (0.15–0.34%). The wide-angle X-ray diffraction results revealed the amorphous nature of copolymers. The copolymer PEIBI-80 showed good balance in solubility, thermal and mechanical properties.
研究领域:
材料科学
·
高分子化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yehan Xiong,Tiantian Xu,Bingchang Chen,Jiangkun Du,Lijing Tan,Yujie Zhong,Jianguo Bao
The photocatalytic performance of materials is primarily governed by their band structure, charge carrier transport, and active sites. This study introduces a surface modification strategy for graphitic carbon nitride (g-C 3 N 4 ) using C=O groups to significantly enhance its photocatalytic activity. The C=O-modified g-C 3 N 4 (CNSHQC2) demonstrated exceptional photocatalytic performance. It achieved a degradation rate of over 85 % for tetracycline hydrochloride (TC) in five different real wastewater matrices within 40 min of natural sunlight exposure. By combining quantitative structure-activity relationship analysis with site-specific blocking experiments, the C=O groups were identified as the primary active sites. Traditional functional group modifications typically improve photocatalytic performance by increasing surface area or enhancing charge transfer. In contrast, C=O modification simultaneously optimizes the band structure and introduces active sites that promote PMS activation. The results indicate that this dual modulation of electronic structure and surface chemistry facilitates efficient charge carrier separation and enhances the generation of reactive oxygen species (ROS). Additionally, C=O groups increase triplet exciton generation and promote singlet oxygen formation via energy transfer. These synergistic effects collectively contribute to a significant improvement in the photocatalytic performance of g-C 3 N 4 . This work provides a new strategy for designing high-performance photocatalysts and valuable insights into the role of C=O groups in expanding the potential applications of carbon-based materials in environmental remediation.
研究领域:
环境科学
·
材料化学
·
光催化
·
水环境修复
·
纳米材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Zong-Pin Fu,Qi-Jie Zhou,Yun-Peng Zhao,Yu-Fa Wu,Fang-Jing Liu,Mei Zhong,Jian Li,Jing Liang,Jing-Pei Cao
The abundant bridging bonds and side chains in lignin make the selective cleavage of its C-O bonds a promising approach for achieving efficient conversion. Herein, Cu/CoOx-CeO 2 catalysts were prepared and the effects of their physical and chemical structures on C-O bond hydrogenolysis activity were investigated. The results indicated that incorporating an appropriate amount of CeO 2 as a support facilitated the doping of Co n+ cations into the CeO 2 lattice, enhancing oxygen vacancy concentration. Additionally, the Cu K-edge X-ray absorption near-edge structure (XANES) spectra revealed that Cu exists in a mixed valence state (Cu δ+ , 0 < δ < 2) within the catalyst. Reaction pathway regulation was achieved through strategic modulation of reaction conditions. When isopropanol was used as the solvent under a N 2 atmosphere, 2-phenoxy-1-phenylethanol (2-PPE-ol) was completely converted at 180 °C within 2 h, yielding ethylbenzene and cyclohexanol with 100 % selectivity. Conversely, when n -hexane was employed as the solvent, dehydrogenation of the C α -OH group generated hydrogen radicals, which promoted cleavage of the C β -O bond in the β-O-4 ketone intermediate, resulting in phenol and 1-phenylethanol with 100 % selectivity. Isotopic labeling and active hydrogen tracking experiments revealed that the active hydrogen in catalyst transfer hydrogenolysis (CTH) originated from the solvent, whereas self-hydrogen-transfer hydrogenolysis (SHTH) relied on hydrogen derived from the C α -OH group of 2-PPE-ol. This work provides valuable insights into the directional conversion of lignin into high-value chemicals and efficient energy utilization.
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DOI
高影响因子
ENERGY & FUELS
·
2026
·
IF 5.3
Chuang Zhang,Yue Wang,Xin Hu,Wei Jiang,Xiao-Yan Zhao,Chen Xu Chen,Wen Li,Jing-Pei Cao
Selective hydrogenolysis of C–O bonds in lignin is widely regarded as the most promising strategy for generating high-value chemicals and clean liquid fuels. Ni–Ru bimetallic catalyst supported on solid superacid was successfully synthesized and applied to the cleavage of C–O bonds in diphenyl ether (DPE) and alkali lignin. The catalytic hydrogenolysis of DPE over a 10%Ni–0.5%Ru–S2O82–/ZrO2 catalyst produced 88.0% cyclohexanol. Additionally, 10%Ni–0.5%Ru–S2O82–/ZrO2 catalyzed the depolymerization of alkali lignin in high yields of phenolic compounds, primarily including guaiacol and methoxyphenol. The synergistic effect between Ni and Ru promoted electron transfer from Ni to Ru. The incorporation of Ru improved the dispersion of Ni and reduced the average particle size of metallic Ni. The strong acidity of the solid superacid support provided abundant acidic sites, facilitating hydrogen atom adsorption and thereby promoting C–O bonds cleavage.
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Qibin Zeng,Yuancai Lv,Meiyan Shi,Ting Pan,Yunhe Xie,Yifan Liu,Minghua Liu
Selective cleavage of C-O bonds is a pivotal step for converting lignin into value-added chemicals, yet the development of efficient catalysts for mild-conversion remains a formidable challenge. Herein, a novel bi-Ni metal catalyst (Ni NPs-SAs /NC) composing of Ni single atoms (SA) and Ni nanoparticles (NP) was synthesized by pyrolysis strategy and employed for lignin hydrogenolysis without external hydrogen gas. Due to the high reactivity of Ni NPs-SAs /NC, various lignin model compounds (α-O-4, β-O-4 and 4-O-5, etc.) were fully converted into aromatic monomers at low temperature (200 ℃) and autogenous pressure, and the selectivity of aromatic monomers was as high as 86.3 %. Structural characterization and theoretical calculations indicated that the excellent catalytic performance of Ni NPs-SAs /NC catalysts was attributed to the synergistic effect of Ni SA and NP sites. Specifically, isopropanol was adsorbed at the Ni NP site and generates active hydrogen, and the Ni SA site adsorbed and activated the C-O bonds. The active hydrogen spillover from the Ni NP site to the Ni SA site enabled the cleavage of the C-O bond of lignin under mild conditions. This work may pave the way for developing high-performance non-noble metal catalysts with exceptional reactivity and selectivity for the valorization of lignin.
研究领域:
催化
·
可再生能源
·
生物质转化
·
材料化学
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Ying Kang,Xingmei Lu,Junli Xu,Qing Zhou,Guangjin Zhang,Jiayu Xin,Dongxia Yan,Ibrahim E.I. Tantawy E.I. Sayed
Transforming lignin into aromatic monomers is critically attractive to develop green and sustainable energy supplies. However, the usage of the additional catalysts like metal or base/acid is commonly limited by the caused repolymerized and environmental issues. The key step is to mediate electron transfer in lignin to trigger lignin C-C/C-O bonds cleavage without the catalysts mentioned above. Here, we report that the ionic liquids [BMim][ClO 4 ] was found to trigger lignin electron transfer to cleave the C-C/C-O bonds for aromatic monomers without any additional catalyst. The proton transfer from [BMim] + to [ClO 4 ] − could polarize the anion and decrease its structure stability, upon which the active hydroxyl radical generated and induced lignin C-C/C-O bonds fragmentation via free radical-mediated routes with the assistance of photothermal synergism. About 4.4 wt% yields of aromatic monomers, mainly composed of vanillin and acetosyringone , are afforded in [BMim][ClO 4 ] under UV-light irradiation in the air at 80 °C. This work opens the way to produce value-added aromatic monomers from lignin using an eco-friendly, energy-efficient, and simple route that may contribute to the sustainable utilization of renewable natural resources.
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PubMed
高影响因子
危险品化学品经营许可证（带存储）