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AICHE JOURNAL · 2025 · IF 4

Hierarchical catalysts with controllable C?C and C?O bond activation ability for selective hydrogenation of oleic acid

Jinlin Mei,Zhentao Liu,Zhengkai Cao,Aocheng Wang,Xiaoyang Kong,Aijun Duan,Chunya Wang,Chunming Xu,Xilong Wang

Hierarchical Y/SBA-15 meso-microporous composites (YS- x ) and corresponding highly dispersed catalysts (Ni/YS- x ) were prepared and applied to the production of jet fuel range hydrocarbons by the selective hydrogenation of oleic acid. Small particle size and electron-deficient Ni δ+ are detrimental to the C  C bond activation of the η 1 (C)-acyl conformation and inhibit the decarbonylation/decarboxylation pathway. Besides, the activation ability of the C  C bond is regulated to avoid excessive cleavage by the acidity and diffusion properties of the hierarchical Ni/YS- x catalysts, thus affecting their hydroisomerization and hydrocracking properties. The abundant acid sites are beneficial to the selective activation of the C  O bond of the η 2 (C, O)-aldehyde conformation and the promotion of the reductive deoxygenation pathway. The optimal Ni/YS-1 shows the highest iso / n -alkane ratio ( i / n = 6.26) and superior jet fuel range hydrocarbons yield (48.8%, 340°C), which is a benefit from its outstanding acid–metal balance and worthy diffusion property.

研究领域: 催化 · 多孔材料 · 化学反应工程 · 能量转换 · 表面化学
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Journal of Physical Chemistry C · 2012 · IF 4.805

Fabrication of Te@Pd Core–Shell Hybrids for Efficient C–C Coupling Reactions

Yuewu Zhao,Huile Jin,Huan Zhou,Juanjuan Lin,Shun Wang,Jichang Wang

Te@Pd core–shell hybrids were prepared in this study, in which a pine leaf-shaped microstructure was obtained through controlling the synthesis kinetics of single crystal Te. The as-prepared Te was subsequently utilized as the substrate for Pd coating. These core–shell particles were characterized with scanning and transmission electron microscopy, high resolution transmission electron microscopy, X-ray diffraction, and energy dispersive X-ray spectroscopy. When being applied as a catalyst in bromobenzene and phenylboronic acid reaction, 100% conversion of bromobenzene was achieved in less than 3 h, which was much shorter than that required by the reactions using graphene oxide supported Pd catalyst (4 h) or the commercial Pd/C catalyst (>6 h). The Te@Pd core–shell catalyst could be easily recovered from the reaction solution and be used repeatedly. The high catalytic activity of Te@Pd hybrids is attributed to their unique microstructure.

研究领域: 材料科学 · 催化化学
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International Journal of Applied Ceramic Technology · 2023 ·Vol. 20 ·期 6 ·3635-3646 · IF 2.1

Oxidation-induced crack-healing behavior of SiC-Al2O3-TiB2 composites at 600°C–800°C

Haopeng Cai,Yinglong Wei,Baoguo Wang,Kun Jiang

It is necessary to give self-healing function to ceramic materials because of their notch sensitivity. In the past, studies on self-healing ceramics have mainly focused on the high-temperature stage, and less research has been done below 1000°C. In this study, SiC/Al 2 O 3 /TiB 2 ceramic composites were prepared by spark plasma discharge sintering, and cracks were introduced on the surface of the polished specimens. Crack healing at 600°C–800°C was investigated, and the recovery of macroscopic bending strength and the change of microscopic crack morphology after heat treatment were used to evaluate the crack-healing effect. It was found that the surface cracks of the material were completely filled and healed by oxidation products after heat treatment at 700°C for 60 min, and the highest healing efficiency exceeded 95% for both specimens with different crack lengths, and the main mechanism of crack by Si-Al-B-Na-Ca-O type glass produced by the reaction of TiB2 and a small amount of SiC with oxygen to produce oxides and glass powder. Good healing effect and fast healing speed effectively improve the service life and reliability of ceramic materials, which has very far-reaching significance for the practical application with ceramic materials.

研究领域: 材料科学 · 陶瓷工程
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA · 2023 ·Vol. 120 ·期 44 ·e2307320120 · IF 11.1

Boosted C–C coupling with Cu–Ag alloy sub-nanoclusters for CO2-to-C2H4 photosynthesis

Yangyang Yu,Ye He,Ping Yan,Shengyao Wang,Fan Dong

The selective photocatalytic conversion of CO2 and H2O to high value-added C2H4 remains a great challenge, mainly attributed to the difficulties in C–C coupling of reaction intermediates and desorption of C2H4* intermediates from the catalyst surface. These two key issues can be simultaneously overcome by alloying Ag with Cu which gives enhanced activity to both reactions. Herein, we developed a facile stepwise photodeposition strategy to load Cu–Ag alloy sub-nanoclusters (ASNCs) on TiO2 for CO2 photoreduction to produce C2H4. The optimized catalyst exhibits a record-high C2H4 formation rate (1110.6 ± 82.5 μmol g−1 h−1) with selectivity of 49.1 ± 1.9%, which is an order-of-magnitude enhancement relative to current work for C2H4 photosynthesis. The in situ FT-IR spectra combined with DFT calculations reveal the synergistic effect of Cu and Ag in Cu–Ag ASNCs, which enable an excellent C–C coupling capability like Ag and promoted C2H4* desorption property like Cu, thus advancing the selective and efficient production of C2H4. The present work provides a deeper understanding on cluster chemistry and C–C coupling mechanism for CO2 reduction on ASNCs and develops a feasible strategy for photoreduction CO2 to C2 fuels or industrial feedstocks.

CAS / MDL: 10031-43-3 7761-88-8
研究领域: 化学 · 材料科学 · 环境科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2020 · IF 4.65

Yolk-double shell Fe3O4@C@C composite as high-performance anode materials for lithium-ion batteries

Xuhui Wang,Jianying Wang,Zihe Chen,Kai Yang,Zexian Zhang,Zhuoxun Shi,Tao Mei,Jingwen Qian,Jinhua Li,Xianbao Wang

Herein, yolk-double shell Fe 3 O 4 @C@C nanospheres (YDS-FCCNs) were designed and synthesized via solvothermal and following heat management. The as-obtained yolk-shell morphology consisted by two parts: one for the Fe 3 O 4 @C nanosphere (diameter about 100 nm) as core, and the other for nitrogen-doped carbon (thickness about 50 nm) as the shell. The YDS-FCCNs composite exhibited preeminent cycling stability of 780 mAh/g at 0.5 A/g after 500 cycles, even at higher current density of 2 A/g, it still retained a reversible capacity of 559 mAh/g after 500 cycle. The good electrochemical performance could attribute to the following factors: First, the hierarchical double carbon shell could prevent the agglomeration of the Fe 3 O 4 , meanwhile largely enhance the electrical conductivity . Second, the synergistic effects for multilayered structure and atomic doping could improve the comprehensive electrochemical performance.

研究领域: 材料科学 · 能源存储
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ChemSusChem · 2020 ·Vol. 13 ·期 19 ·5248-5255 · IF 7.962

Metal-free Photocatalytic Aerobic Oxidative Cleavage of C−C Bonds in 1,2-Diols

Rui Zhu,Gongyu Zhou,Jia-nan Teng,Xinglong Li,Yao Fu

Graphical Oxidative cleavage : A heterogeneous metal-free photocatalytic system is developed for oxidative cleavage of C−C bonds in 1,2-diols at mild conditions (visible light, room temperature, no base, O 2 balloon). The reaction mechanism is studied through a series of control experiments and DFT calculations. In addition, the catalytic system has a broad substrate scope, including aliphatic, benzylic, alkenyl 1,2-diols, and α-hydroxy acids such as lactic acid. The preparation of carbonyl compounds by the aerobic oxidative cleavage of C−C bonds in 1,2-diols under mild reaction conditions is a very significant reaction and is widely employed in various scenarios. Avoiding the use of harmful stoichiometric oxidants and adopting a greener chemical process remain a challenge for this reaction to date. In this manuscript, a heterogeneous metal-free photocatalytic strategy without any additive was developed for aerobic oxidative cleavage of C−C bonds in 1,2-diols at ambient conditions with visible light. The reaction mechanism was further studied through a series of control experiments and density functional theory (DFT) calculations. In addition, the catalytic system showed a broad substrates scope, including aliphatic (linear or cyclic) 1,2-diols, benzylic, alkenyl 1,2-diols, and α-hydroxy acids (such as lactic acid). Thus, this strategy could serve as a method for the transformation of 1,2-diols to corresponding carbonyl compounds by the aerobic oxidative cleavage of C−C bonds.

研究领域: 有机化学 · 催化化学 · 环境化学
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RSC Advances · 2016 ·Vol. 6 ·期 76 ·72744-72749 · IF 3.289

Catalytic oxidative C–C bond cleavage route of levulinic acid and methyl levulinate

Fei Xia,Zhongtian Du,Junxia Liu,Yangyang Ma,Jie Xu

Recently, obtaining value-added chemicals from biomass resources has attracted considerable attention. Levulinic acid is one of the most important biomass platform compounds, which could be obtained from carbohydrate biomass. In this work, levulinic acid was selectively converted into C4 product, including succinic anhydride, via catalytic oxidation with a manganese catalyst in acetic anhydride. Moreover, an unexpected product of maleic anhydride was obtained, which greatly differs from that of levulinate ester. The pathway for formation of maleic anhydride was studied by monitoring and confirming intermediates α-angelica lactone and its derivative 2-methyl-5-oxotetrahydro-2-furanyl acetate. Based on the obtained mechanistic information, the different behaviour between the oxidative cleavage of levulinic acid and levulinate ester was further discussed.

研究领域: 化学工程 · 可再生资源化学
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BIOMACROMOLECULES · 2020 · IF 6.092

Dynamic Covalent C═C Bond, Cross-Linked, Injectable, and Self-Healable Hydrogels via Knoevenagel Condensation

Caicai Jiao,Lilong Gao,Hui Zhang,Bing Yu,Hailin Cong,Youqing Shen

Hydrogels have a wide range of applications in the fields of biomedicine, flexible electronics, and bionics. In this study, injectable and self-healable hydrogels were first prepared based on a dynamic covalent C═C bond formed via the Knoevenagel condensation reaction between poly(ethylene glycol) dicyanoacetate and water-soluble poly(vanillin acrylate). Three kinds of catalysts (phosphate buffer, zeolitic imidazolate framework-8, and tertiary amine) were used in Knoevenagel condensation for preparing hydrogels. All hydrogels in this study could be formed in situ, and their gelation time ranged from seconds to minutes. The properties and application of hydrogels could be customized according to the type of catalyst employed. 3-[4,5-Dimethylthiazol-2-yl]-2,5-diphenyltetrazolium bromide (MTT) results indicated that all the components and hydrogels exhibited low toxicity, and the hydrogels could be used as 3D cell culture scaffolds. Because of the dynamic covalent C═C bond formed by Knoevenagel condensation, the resultant hydrogels were found to be dynamic and showed good self-healing properties. This work presents a new dynamic covalent chemistry for the preparation of self-healable materials.

研究领域: 生物医学工程 · 材料科学 · 组织工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Visible-light driven phosphotungstic acid/tubular C3N4 heterojunction photocatalyst for efficient cleavage of C–C bond in lignin

Song Han,Yun Zhao,Mina Liang,Jinshui Su,Xiangxiong Zhai,Qi Zhang,Guoling Li,Zhonghai Ni

The photocatalytic cleavage of C α -C β bonds in lignin holds considerable potential for the production of value-added chemicals. Lignin consists of phenylpropane units interconnected by a variety of complex chemical bonds. Specifically, C-O bonds are more prevalent and relatively easier to cleave, whereas C–C bonds exhibit higher bond energy, rendering them more difficult to cleavage under conventional conditions. This study presents a phosphotungstic acid/phosphoric acid-functionalized porous tubular C 3 N 4 composite photocatalyst (PW/P-TCN). H 3 PO 4 modified PW/P-TCN surfaces enhance O 2 adsorption, improve separation and transfer of photogenerated carriers, and increase exposure of active sites. This promotes reactant adsorption and significantly boosts photocatalytic efficiency. Through this strategy, 1,2-diphenylethanol (DPol), used as a typical model substrate, is fully converted into aromatic monomers, achieving a DPol conversion rate of 99.9 %. Mechanistic studies reveal that C α -C β bond cleavage primarily involves the photo-oxidation mechanism mediated by electron-hole coupling. The construction of the PW/P-TCN heterojunction is essential for simultaneously sustaining robust reduction and oxidation capabilities. Natural lignin samples are applied to the photocatalytic system, and successful C–C bond cleavage depolymerization is achieved under optimal reaction conditions. This study offers valuable insights for the design of more economical and efficient photocatalysts for lignin depolymerization.

研究领域: 材料科学 · 环境科学 · 化学工程
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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Simultaneous Differentiation of C═C Position Isomerism in Fatty Acids through Ion Mobility and Theoretical Calculations

Fangling Wu,Xishi Wu,Chaoxian Chi,Chuan-Fan Ding

Fatty acids play a pivotal role in biological processes and have many isomers, particularly at the C═C position, that influence their biological function. Distinguishing between isomers is crucial to investigating their role in health and disease. However, separating the isomers poses a significant analytical challenge. In this study, we developed a simple and rapid strategy combining ion mobility spectrometry and theoretical chemical calculations to differentiate and quantify the C═C positional isomers in 2-/3-butenoic acid (BA), 2-/3-/4-pentenoic acid (PA), and 2-/3-/5-hexenoic acid (HA). C═C positional isomerism was mobility-differentiated by simple complexation with crown ethers (12C4, 15C5, and 18C6) and divalent metal ions (Mg2+, Ca2+, Mn2+, Fe2+, Co2+, Ni2+, Zn2+, Sr2+, and Ba2+), that is, converting C═C positional isomers with small structural differences into complexes with large structural differences through the interaction with metal ions and crown ethers. Metallized isomers were formed but could not be differentiated due to their complex and overlapping extracted ion mobiliograms (EIMs). Binary crown ether–isomer complexes were not observed, indicating that C═C positional isomers could not be separated by simple mixing with crown ethers. However, significant EIM differences were obtained for the formed ternary complexes, allowing baseline separation for the isomers. Notably, all crown ethers and metal ions have a separation effect with the isomers, with a calculated separation resolution (Rp–p) of 0.07–2.44. Theoretical chemical calculations were performed to provide in-depth structural information for the complexes and explain the separation principle. Theoretical conformational space showed that the divalent metal ions act as a bridge connecting the crown ether and the isomer. Additionally, the ternary complex becomes more compact as the distance between C═C and −COOH increases. Theoretical results can reflect the features of mobility experiments, with relative errors between the experiment collision cross-section (CCS) and theoretical CCS of no more than ±8.06%. This method was also evaluated in terms of quantification, accuracy, and precision repeatability. Overall, this study establishes that the crown ether–metal ion pair can function as a robust unit for differentiating C═C positional isomerism.

研究领域: 分析化学 · 生物化学
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Journal of Physical Chemistry C · 2025 · IF 3.2

Suppressing Reverse Radical Conversion via Diluting Local Hydrogen Ions for Efficient Photocatalyzed C–C Coupling between Benzyl Alcohol and Benzaldehyde

Xiang Chen,Shaohua Chen,Pengxin Liu,Chaodan Pu

We report the efficient C–C coupling between benzyl alcohol and benzaldehyde to hydrobenzoin using CdSe/CdS quantum dots as visible-light photocatalysts and sodium oxide as a cocatalyst. The optimized conditions resulted in a reaction with a selectivity of hydrobenzoin >95%, an apparent quantum yield of 23.6% under the excitation by 520 nm LED, and a turnover frequency of 56.8 mmol g–1 h–1. Reactant concentration-dependent experiments demonstrated that benzaldehyde can process fast proton-coupled electron transfer, improving the utilization of photogenerated electrons. Photoluminescence quenching experiments and reactions with deuterated benzaldehyde confirmed that due to the in situ produced hydrogen ions, the hydroxymethyl radicals would process efficient reverse conversion from hydroxymethyl radicals to benzyl alcohol, resulting in noneffective charge transfer. Formation of sodium benzyloxide can eliminate the in situ produced hydrogen ions around the hydroxymethyl radical, suppressing this reverse conversion and improving the utilization efficiency of transferred holes and electrons.

CAS / MDL: 10108-64-2 3317-61-1
研究领域: 化学 · 材料科学
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ANALYST · 2022 ·Vol. 147 ·期 7 ·1341-1347 · IF 5.227

Electrochemically activated carbon–halogen bond cleavage and C–C coupling monitored by in situ shell-isolated nanoparticle-enhanced Raman spectroscopy

Chen-Chen Jiang,Xiao-Chong Li,Jian-Ang Fan,Jia-Ying Fu,Xu-Nan Huang-Fu,Jia-Jie Li,Ju-Fang Zheng,Xiao-Shun Zhou,Ya-Hao Wang

The electroreductive cleavage of carbon–halogen bonds has attracted increasing attention in both electrosynthesis and pollution remediation. Herein, by employing the in situ electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) technique, we have successfully investigated the electroreductive dehalogenation process of aryl halides with the thiol group on a smooth Au electrode in aqueous solution at different pH values. The obtained potential-dependent Raman spectra directly reveal a mixture of the reduction products 4,4′-biphenyldithiol (BPDT) and thiophenol (TP). The conversion ratios of the C–Cl and C–Br bonds at pH = 7 are 37% and 55%, respectively. Furthermore, quantitative analysis of the intensity variations of ν(C–Cl), ν(C–Br) and aromatic ν(CC) stretching modes suggests electroreductive dehalogenation via both direct electron transfer reduction and electrocatalytic hydrodehalogenation. Molecular evidence for the C–C cross coupling process through TP reaction with benzene free radical intermediates is found at negative potentials, which leads to the increasing selectivity of biphenyl products.

CAS / MDL: 106-53-6 106-54-7
研究领域: 电化学 · 材料科学 · 环境科学
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