ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Haoze Li,Mengyao Wang,Yingbing Zhang,Ye Chen,Li Wang,Jianping Yang
The photoreforming of plastic waste into high-value chemicals and H 2 fuels presents a sustainable and energy-efficient strategy to mitigate environmental pollution and energy crises. However, achieving high selective valuable products remains challenging due to the indiscriminate cleavage of chemical bonds in plastics. Herein, this study reports a sulfur-vacancies-rich ZnIn 2 S 4 photocatalyst decorated with ultrafine Ni nanoparticles (Ni 0.2 @ZIS-S v ) that enables highly photoreforming of poly(ethylene terephthalate) (PET) into formate and H 2 via targeted C─C bond cleavage under mild alkaline conditions. The Ni 0.2 @ZIS-S v photocatalyst achieves an H 2 evolution rate of 4.5 mmol g −1 h −1 , a 20.2-fold enhancement over pure ZnIn 2 S 4 , while formate is the primary liquid product with the selectivity reaching 84.8%. Mechanistic analysis reveals that the combined effects of Ni nanoparticles and sulfur-vacancies modify the electronic structure of ZnIn 2 S 4 , improving charge separation, lowering the energy barrier for H 2 generation, and facilitating selectively C─C bond cleavage. This dual optimization enhances both hydrogen yield and formate selectivity, demonstrating an effective strategy for designing advanced photocatalysts to upcycle plastic waste into high-value chemicals and clean energy.
研究领域:
光催化化学
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环境催化
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能源材料
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高分子降解
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清洁能源转化
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·Vol. 14
·期 14
·4058-4067
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IF 4.4
Yang You,Aijie Xu,Yao Lv,Lide Yang,Xuan Tang,Jie Tang,Yanglong Guo,Yao Cui,Wangcheng Zhan,Li Wang,Yun Guo,Sheng Dai
Complete oxidation of propane has drawn great attention in the fields of automotive emission control and volatile organic compound elimination. However, it is challenging to achieve high activity of this reaction due to the stability of propane. We here utilize a facile solvothermal method to construct tri-coordinated Al (AlIII) sites on the as-synthesized ST-Al2O3 support to alter the properties of supported Pt species. It is demonstrated that AlIII sites facilitate the dispersion and electron enrichment of supported Pt sites. Thus, Pt/ST-Al2O3 exhibits a superior activity toward complete propane oxidation, showing a 6.7-fold improvement in the turnover frequency over commercial Pt/Al2O3 catalysts. Meanwhile, Pt/ST-Al2O3 possesses a distinct reaction route originating from its stronger C–H and C–C cleavage capability, while having excellent activity not only in complete propane oxidation but also in the complete oxidation of other alkanes (CH4, C2H6, and n-C4H10). In addition, the AlIII construction strategy is successfully extended to more cases, e.g., Pd/ST-Al2O3 with higher Pd dispersion and electron density. This work provides a promising strategy for the control of the oxide support for advanced design and synthesis of alkane oxidation catalysts.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
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2024
·Vol. 14
·期 4
·973-979
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IF 4.4
Peidong Ren,Lei Shi,Ziwang Kan,Jiaxiao Bai,Yunyi Liu,Shucheng Yang,Siqi Li,Song Liu
The electrochemical conversion of lignin for the production of high-value aromatic compounds holds immense potential. However, the process of depolymerizing lignin faces significant challenges due to its intricate structure, particularly the existence of C–C bonds, resulting in low conversion and product yields. In this work, we report the successful synthesis of a molecular palladium catalyst and its inaugural application in the electrochemical conversion of lignin model compounds. This catalyst with well-defined coordination structure demonstrates exceptional efficacy and achieves a remarkable 99% conversion rate for the lignin model compound 2-phenoxy-1-phenylethanol with a yield of 32% of the benzaldehyde product while valuable hydrogen is produced at the electrode under ambient conditions. Furthermore, employing radical trapping and EPR test point that the tBuO˙ radical was the key to inducing C–C cleavage for high conversion and enabled a comprehensive elucidation of the possible reaction pathways involving radical/radical cross-coupling. Based on this study, we believe that molecular catalysts will open a new chapter in the electrocatalytic conversion of lignin.
研究领域:
化学
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能源科学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
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2024
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IF 9.3
Hao Huang,Guangping Zhou,Min Zhuang,Xiaolan Cai,Shaoqu Xie
Bioenergy is a key strategy for sustainability, yet the potential for biofuel production from chitin is under-exploited. Here, we report the cleavage of the inherently inert σ-type C-C bonds in chitin under the condition of initially breaking the unstable C-O bonds. Mechanistic studies indicate that by regulating the valence state of Ru and the interaction between RuOx and AC-HNO3-melamine, the ability of Ru nanoparticles to cleave C-C and C-O bonds can be controlled. One-pot sequential hydrogenolysis of chitin with RuOx/AC-HNO3-melamine resulted in a mixed alcohol yield 1.66 times that of commercial Ru/C. A mixed alcohol yield of 16.8% was achieved using raw chitin and green process conditions. We expanded the substrate range to include chitosan, N-acetyl-D-glucosamine, and glucosamine. This work demonstrates the potential of marine biomass to produce affordable clean energy.
研究领域:
化学工程
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生物技术
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
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2014
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IF 3.309
Junjie Zhang,Fang Lu,Weiqiang Yu,Jiazhi Chen,Shuai Chen,Jin Gao,Jie Xu
The use of high pressure fossil derived hydrogen limits the commercial prospects of transforming sorbitol to glycols. Ni–Re/C catalyst which was developed in this study demonstrated high selectivity toward hydrogenative cleavage of C2–C3 and C3–C4 bonds of sorbitol to produce glycols under 1 MPa nitrogen. Acetol which is proposed as important intermediate to explain the reaction mechanism was first detected in the sorbitol conversion reactions. Detailed investigations showed that the presence of Re could prevent the sintering of Ni particles during the reduction process and make the catalyst efficiently generate hydrogen on the active sites to selectively cleave C–C bonds in sorbitol under nitrogen atmosphere.
研究领域:
催化化学
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绿色化学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2019
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IF 6.97
Wenwen Qiang,Xiang Liu,Teck-Peng Loh
The first example of a heterogeneous catalyst based on hydrotalcite-derived Mg–Al oxides supported iridium (Ir/MgxAlO) for activation of methanol in the synthesis of bis(indolyl)methanes (BIMs) is reported. In this clean and reusable iridium-based catalytic system, a variety of substituted indoles were selectively converted to their corresponding BIMs in moderate to good yields with high tolerance to reducible functional groups by using methanol as a bridging methylene (−CH2−) donor. The high catalytic activity and selectivity of the reaction benefit from the delicate cooperation of redox/acid–base surface sites on this artificially designed multifunctional Ir/MgxAlO catalyst. The overall simplicity, chemoselectivity and sustainability of the catalytic system make this approach a valuable and step-economical tool to construct C–C bond directly from methanol in the synthesis of more complex molecules.
研究领域:
化学
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催化材料科学
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DOI
高影响因子
NANOTECHNOLOGY
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2024
·Vol. 35
·期 49
·495704
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IF 2.9
Gang Xiao,Zishuai Wang,Yu Jin,Fengping Wang
The selective cleavage of lignin C–C bonds is a highly sought-after process with the goal of obtaining low-molecular-weight aromatic chemicals from renewable resources. However, it remains a challenging task to achieve under mild conditions. Photocatalysis is a potentially promising approach to address this issue, but the development of efficient photocatalysts is still in progress. In this study, we introduce the heterostructured TiO2@g-C3N4 photocatalyst for the development of a visible light photocatalytic procedure for the selective cleavage of lignin C–C bonds under mild conditions. The photocatalyst displays favourable visible light absorption, efficient charge separation efficiency, and promising reusability. A typical β–O–4 dimer model, 2-phenoxy-1-phenylethanol, was effectively (96.0% conversion) and selectively (95.0 selectivity) cleaved under visible light at ambient conditions. This photocatalytic procedure was also effective when subjected to solar irradiation or other lignin dimer models with β–O–4 or β-1 linkages. This reaction occurred through a Cβ-centred radical intermediate and a six-membered transition state with photogenerated holes as the primary active species. The Cα–OH oxidative dehydrogenation of the substrate could also take place but was a relatively minor route. This study provides a new photocatalytic procedure for visible-light-driven lignin valorisation and sheds light on the design of high-performance nanocomposite photocatalysts for C–C bond cleavage.
研究领域:
化学工程
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材料科学
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可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RARE METALS
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2025
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IF 11
Dong Yu-Guo,Kong Wen-Jing,Ma Zhuang,Yang Yong,Wang Ping,Sheng Shi-Xiong,Dong Lin,Gu Xiao-Li,Chen Zu-Peng
The oxidation of lignin model compounds to esters via C–C bond cleavage has attracted considerable attention, as esters could be used as important polymer precursors and pharmaceutical intermediates. However, most studies focus on designing homogeneous or noble metal catalysts and conducting the reactions under basic conditions. Here, we report an efficient process for the C–C bond cleavage of lignin model compounds and selectively producing esters over different shaped CeO 2 (i.e., nanospheres (S), nanorods (R), nanoparticles (P), and nanocubes (C)) under base-free conditions. Specifically, the yield of methyl anisate from the aerobic oxidation of 1-(4-methoxyphenyl)ethanol reaches 77.6% over CeO 2 -S in one hour (91% in 9 h), exhibiting higher performance compared to other evaluated CeO 2 catalysts (6.4%–40.2%). Extensive characterizations and experimental investigations reveal that the density of weak base sites and oxygen vacancies on the CeO 2 surface is positively correlated with the yield of methyl esters. Furthermore, the reaction pathway is investigated, which confirms that 1-(4-methoxyphenyl)ethanol first undergoes two reactions (i.e., etherification and dehydrogenation) to produce intermediates of 1-methoxy-4-(1-methoxy-ethyl)-benzene and 1-(4-methoxyphenyl)ethanone, respectively, followed by a series of functional group transformations to generate the targeted methyl anisate ultimately. Graphical abstract
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
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2025
·
IF 6.3
Ting Li,Jiantao Bi,Huajing Li,Qing Li,Yuangang Li
The synergistic coupling of photocatalytic C C bond construction and H 2 evolution presents a promising strategy for concurrent organic synthesis and sustainable H 2 evolution. Nevertheless, precisely regulating the reaction pathways to enhance the selectivity of target products remains a challenging. Here, the Sv-CdS/TiO 2 Ni 2 P photocatalyst containing sulfur vacancies was synthesized via calcination, achieving highly selective conversion of 4-pyridinemethanol into the C C coupling product 1,2-di-(4-pyridyl)-1,2-ethanediol under visible-light irradiation, with a selectivity of 96.59 %. In comparison, the M-CdS/TiO 2 Ni 2 P photocatalyst prepared by mechanical mixing exhibits superior H 2 evolution activity of 6.48 mmol·g -1 ·h -1 . Mechanism studies reveal that 4-pyridinemethanol interacts with the Sv-CdS/TiO 2 Ni 2 P photocatalyst through the N atom, which preferentially activates the sp 3 C H bond of 4-pyridinemethanol to generate •CH(OH)C 5 H 4 N radical for further C C coupling reaction. This work not only highlights the selective regulation of the 4-pyridinemethanol C C coupling pathway by sulfur vacancies engineering, but also provides new insights for achieving efficient photocatalytic organic synthesis and green H 2 evolution.
研究领域:
光催化
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有机合成
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材料科学
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环境化学
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能量转换
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Ajibola T. Ogunbiyi,Wenzhi Li,Leyu Zhu,Amir Hamza,Jingting Jin
Despite lignin’s massive potential for biobased clean fuel production, developing effective catalysts for selectively cleaving its interunit bonds to harness this potential continues to be challenging. In this study, an HZSM-5-supported MoO3 catalyst was developed for a one-pot, hydrothermal kraft lignin depolymerization to maximize liquid fuel yield. A record-high 85.1% yield of petroleum ether-soluble product (a potential gasoline substitute), an unprecedented 45.3% yield of aromatic monomer, and a meager 4.9% char yield (corresponding to a 95.1% lignin conversion) were realized at 300 °C and 24 h in a catalytic transfer hydrogenolysis. The resulting liquid fuel afforded a calorific value of 35.97 MJ/kg, significantly improving over the 25.45 MJ/kg in the original kraft lignin. Catalyst characterization results showed that an optimal acidity characteristic and a suitable Mo-zeolite interaction were pivotal to the efficient cleavage of the C–O and C–C bonds in the kraft lignin. The analyses of the spent catalyst revealed that the formation of inactive Mo4+ species and carbonaceous deposits on the catalyst’s surface was responsible for the initial catalyst deactivation, but recalcination reinstated the catalyst activity. This study extends the frontiers of knowledge in rational catalyst development for lignin valorization applications.
研究领域:
催化化学
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生物质能
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
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2022
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IF 5.774
Jie Zhang,Danyang Cao,Shanshan Wang,Xin Feng,Jiahua Zhu,Xiaohua Lu,Liwen Mu
In this study, heteroelement-rich groups (N and B elements, tris (2-hydrazinylethyl) borate) were successfully synthesised on lignin by microwave amination. The reaction between lignin and heteroelement-rich groups was confirmed using several characterization techniques, including fourier transform infrared (FT-IR) spectroscopy, thermogravimetric (TG) analysis, and X-ray photoelectron spectroscopy (XPS). A lignin model compound (2-phenoxyacetophenone (L-M)) was used to study the bond-breaking mechanism of lignin depolymerization , and the amine group, which acted as a nucleophile , attacked the C–C bond to form an amide bond with the lignin. As an effective additive, modified lignin can increase the viscosity of poly (ethylene glycol) 200 (PEG200), reducing the wear volume and friction coefficient in the friction test. Theoretical calculations showed that the polarity of the modified lignin increased, which allowed the modified lignin to form a strong physical adsorption on the metal surface. In addition, the reciprocal hydrogen bonding between the modified lignin and PEG200 contributes synergistically to the enhanced lubrication film strength , and thus, the better tribological properties of these new lubricants.
研究领域:
高分子化学
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材料科学
·
绿色化学
·
表面工程
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能源材料
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可持续技术
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2020
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IF 7.888
Yanru Zhu,Jian Zhang,Xiaodan Ma,Zhe An,Shaowei Guo,Xin Shu,Hongyan Song,Xu Xiang,Jing He
Complexity of chemical linkages (C-C/C-H/C-O, C=C/C=O, or C-O-H/C-O-C) in biomass-derived molecules makes the selective activation of targeted bonds much more challenging, expecting well-defined catalysts and definite catalytically-active sites. This work demonstrates an effective gradient reduction strategy to control the definite structure of catalytically-active sites, affording defects-rich nano-twin Cu particles. This strategy just involves the reduction (calcination under H 2 ) of Cu II -containing layered double hydroxides (LDHs) simply with controlling the reduction gradient (interval time) of Cu II species in two chemical micro-environments (Cu II -O-Cu II and Cu II -O-M II/III/IV (M ≠ Cu)) in the brucite-like layer of LDHs. The nano-twin Cu particles efficiently promote the target activation of C-O and C=C in the conversion of furfural to cyclopentanone (CPO). With ~100% furfural conversion, the defects-rich nano-twin Cu particles afford a CPO selectivity of 92%, 50% higher than regular spherical Cu particles. The multi-stepped defect sites, originating from the planar defects, play a decisive role in promoting the CPO selectivity by facilitating the hydro-deoxygenation to C-O of 4-hydroxycyclopentenone (HCP) and hydrogenation to C=C of HCP or cyclopentenone.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）