ACS Nano
·
2026
·
IF 17.3
Yujun Zhang,Hui Teng,Qingyun Zhi,Xuemei Dong,Yuxiang Mei,Shumin Zhou,Shengwei Ke,Xinghua Yu,Fei Sun,Junmin Zhang
Bimetallic single-atom catalysts (SACs) represent an emerging paradigm beyond single-atom catalysts for enabling synergistic catalysis. The homocoupling of arylboronic acids via C–B bond activation to form C–C bonds has been demonstrated to be entirely inert with Pd or Au SACs. This study achieves a breakthrough by developing a bimetallic single-atom catalyst (Pd1Au1/graphene), which delivers outstanding performance with a TON up to 19,192 and cycling stability (>90% yield after seven cycles). Through comprehensive experiments and theoretical calculations, we have identified a structure of PdN4-AuN4/graphene, where adjacent Pd and Au atoms form a synergistic active center. This promotes simultaneous aromatic boronic acid substrate activation and significantly reduces the reaction energy barrier of the oxidative addition step, thereby enabling a pathway inaccessible to isolated single atoms. This work not only provides an efficient catalyst for organic synthesis but also validates the fundamental principle of synergistic catalysis in bimetallic single-atom catalysts, offering a universal design strategy for addressing challenging transformations.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Kehui Qi,Peng Lu,Xuehui Zhang,Yuxiang Liu,Yue Liu,Lu Li
Single-atom catalysts (SACs) are highly regarded for their high atomic efficiency and outstanding catalytic performance. However, the stable anchoring of single atoms and the precise regulation of their multiple valence states are still challenges. To address this challenge, a structurally stable and valence-tunable multivalent zinc single-atom catalyst was successfully synthesized according to a thermodynamically-driven lattice substitution strategy. Experimental and theoretical analyses indicate that zinc single atoms precisely occupy a pair of adjacent Cu + vacancies in the Cu 2 O lattice with a spacing of approximately 2.9 Å, forming Zn-O-Cu units. This structure establishes an electron transport channel mediated by oxygen bridges, facilitating strong electron coupling between the 3d orbitals of Zn and Cu. This strong coupling results in the formation of a stable multivalent Zn δ+ (0＜δ < 2) state, which is identified as the primary origin of the catalyst’s high activity. Benefiting from the unique electronic synergistic effect of the Zn-O-Cu units and the resulting promotion of oxygen vacancy formation, this catalyst enables carboxylic acid molecules to be adsorbed and activated in a bridging mode. Through this adsorption configuration, the α-C–C bond becomes polarized and significantly weakened, setting the stage for its selective cleavage. The Zn δ+ -O-Cu catalyst showed remarkable catalytic performance in the selective cleavage of the α-C–C bond in fatty acids for alkane production, achieving up to 96.89% n-C n-1 alkane selectivity. Furthermore, the Zn δ+ -O-Cu catalyst demonstrated excellent versatility across fatty acids with varying carbon chain lengths. These results demonstrate the significant promise of this strategy not only for advancing the practical utilization of biomass feedstock with high fatty acid (FA) content, but also for establishing an efficient and novel pathway toward long-chain alkane production.
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ENERGY & FUELS
·
2026
·
IF 6
Tianxiang Guo,Baijiang Liu,Gujie Yao,Xiaoqing Wang,Yanyan Feng,Da Jin,Xilai Wang,Yarong Du
The electrochemical reduction of CO2 to high-value C2 products, especially ethanol, presents a feasible approach for alleviating greenhouse gas emissions and tackling climate-related challenges. Nevertheless, the rational design of efficient electrocatalysts is still restricted by insufficient activity, suboptimal selectivity, and a limited understanding of the underlying mechanisms. In this study, a hierarchically structured Cu-CoPc/CNT catalyst was fabricated by electrochemical deposition and drop-casting techniques. Comprehensive characterization (BET/SEM/XRD/EDS/XPS) confirmed its electronic configuration and surface properties. Electrochemical evaluations (CV/LSV/EIS/GC/1H NMR) demonstrated an ethanol Faradaic efficiency of 42.3% at a partial current density of 10.65 mA·cm–2, with exceptional ethanol selectivity of 98.6% among C2 products at −1.15 V vs RHE. In conjunction with density functional theory (DFT) calculations, mechanistic investigations have demonstrated that an adequate supply of those intermediates such *COOH and the facilitation of the C–C coupling are the primary factors contributing to the performance improvement of the CO2RR toward ethanol through the synergistic effect between CoPc/CNT and Cu. This research proposes a novel strategy for designing efficient and stable CO2-to-ethanol catalysts, thereby deepening the fundamental understanding of the ethanol formation mechanisms.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Zhilun Zhang,Wei Xie,Xuanru Ren,Bingqing Zhao,Ziqi Zhao,Qian Wang,Mingliang Li,Hailong Wang
To enhance oxidation resistance of carbon/carbon (C/C) composite materials at 1973 K in static air, a novel bilayer Yb 2 O 3 -HfB 2 -SiC/SiC (denoted YHSS) coatings were engineered via a two-step process combining pack cementation and slurry method. A substantial loading of ceramic phases (∼60 wt %) was incorporated into the SiC ceramic layer to improve thermal stability of the oxide scale at 1973 K. Following pre-oxidation, the YHSS coatings impart effective oxidation protection to C/C composite materials for over 228 h at 1973 K. Coupled experimental and theoretical analyses confirm that Yb and Hf atoms diffuse into the thermally grown SiO 2 layer, thereby reinforcing the SiO 2 network structure. Furthermore, the coating's exceptional performance is attributed to its dense, flaw-free surface morphology and the homogeneous dispersion of high-content ceramic phases throughout the SiC layer, collectively suppressing oxygen permeation.
研究领域:
材料科学
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陶瓷涂层
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高温材料
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复合材料
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表面工程
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Jin Yuan,Zhiwei He,Hongbo Zhang
Selective C–H bond oxidation of cyclohexane into KA oil (ketone-alcohol) is of vital importance in both fundamental research and industrial applications while limited by complex reaction network and suffering from low efficiency. In this study, Ce(OH)SO 4 · x H 2 O was chosen as a probe to systematically investigate the C–H bond activation and C–C bond rupture as a function of various reaction parameters, including the reactant/product concentrations, catalyst applied, reaction temperatures, acidic concentrations etc, and found that bi-molecule of C 6 H 12 was probably involved in both C–H bond rupture and C–C bond cleavage and both were controlled by one deprotonation elementary step with ·O 2 – and h + as the key active components, which were supported by parity fittings and primary KIEs determined. In addition, the C–C bond rupture was found to be mainly following C 6 H 10 O to ε-caprolactone and further to linear acids reaction path. Hopefully, this study could help people find/optimize reaction systems in selective hydrocarbon upgradings.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2021
·
IF 5.302
Fuhai Liu,Maozhong Yi,Liping Ran,Yicheng Ge,Zhe Zhou,Ke Peng
C/C-BN-SiC composite was prepared by ceramic slurry infiltration combined with resin impregnation and carbonization, and the matrix with continuous distributed self-healing phase was obtained. In this study, the kinetic characteristics and oxidation behavior of the composites with various h-BN/SiC ratios in the temperature range of 600∼1300°C were studied by combining the isothermal oxidation test with the kinetic model. The optimal h-BN/SiC ratio balances the thermal stability and fluidity of the oxidized product, which not only has high thermal stability and low oxygen permeability to acts as an oxygen diffusion barrier but also has a certain fluidity to seal defects.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Xiaoping Zhang,Xiang Ren,Konstantin Chingin,Jiaquan Xu,Xin Yan,Huanwen Chen
We present an approach for the elucidation of C=C bond position and cis/trans isomers, which is achieved by the reaction of ambient water radical cations and double bonds, followed by the fragmentation of epoxide radical cations to generate diagnostic ions in tandem mass spectrometry . Hexenol double bond positional isomers and cis/trans isomers which exhibit different properties and biological functions are characterized as a proof of concept. The merits of the approach include the simplicity of experimental setup, rapid derivatization (within seconds), the obviation of organic solvents , as well as easy spectral interpretation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Rui Li,Qixuan Lin,Yingxiong Wang,Weiran Yang,Xinxin Liu,Weiying Li,Xiaohui Wang,Xiaoying Wang,Chuanfu Liu,Junli Ren
The efficient production of xylose and arabinose from glucose, is significant but technologically challenging. Herein, the conversion of glucose to pentose (xylose and arabinose) and formic acid was realized using non-toxic artificial zeolite and green solvent of γ-butyrolactone-H 2 O. The selective conversion of glucose to 5-hydroxymethylfurfural, pentose and furfural could be regulated by controlling Brønsted acid strength. The weak Brønsted acid could promote the formation of pentose, while strong Brønsted acid could lead to the formation of HMF and further degradation of pentose to furfural. The mechanism was investigated spectroscopically to add fundamental insights to the selective C1-C2 bond cleavage. The solvent of γ-butyrolactone-H 2 O reduced apparent activation energy by promoting the formation of active d -fructofuranose. The favorable yield reached to 54.3 % pentose and 54.7 % formic acid from glucose, while 95.6 % pentose and 96.8 % formic acid from fructose at 453 K for 1.5 h. This strategy offered a new utilization way of glucose in expanding the varieties of platform chemicals.
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 8
·2468-2473
·
IF 9.48
Taimei Cai,Qiang Deng,Hailong Peng,Jin Zhong,Rui Gao,Jun Wang,Zheling Zeng,Ji-Jun Zou,Shuguang Deng
The major challenge in the synthesis of high-density biofuels is to identify the bio-based source for C–C cyclic compounds and C–C coupling reactions with a suitable selectivity. Herein, we selectively synthesize 1,2,4-benzenetriol (BTO) with a yield of 51.4% from cellulose-derived 5-hydromethylfurfural via a ring-rearrangement reaction. The cellulose-derived route is a more meaningful route for the C–C cyclic compounds compared to the traditional hemicellulose- and lignin-derived routes. Furthermore, BTO is very easily dimerized via a C–C oxidative coupling reaction, showing a yield of 94.4% and selectivity of nearly 100% under environmentally friendly reaction conditions. After hydrodeoxygenation, bicyclohexane is obtained with a yield of 87.4%. This work not only provides a promising route to produce C–C cyclic fine compounds based on a cellulose-derived route, but also shows a highly efficient synthesis route for high-density biofuels via the C–C oxidative coupling reaction.
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AICHE JOURNAL
·
2025
·
IF 4
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
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多孔材料
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化学反应工程
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能量转换
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表面化学
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Materials Research Express
·
2025
·Vol. 12
·期 9
·095005
·
IF 2.2
Xinfa Qiang,Xiangyu Chen,Maoheng Dong,Zi Yang,Wensu Meng,Hai Kan,Keqing Wang,Lijin Wang,Ling Wang,Chao Wu
A unique bead-chain-like SiC nanowires (SiCnws) morphology was successfully synthesized via an aerogel carbothermal reduction method. Microstructural analysis revealed that the SiC chain display diameters ranging from 100 to 200 nm, while the SiO2 bead exceed 1 μm in diameter. A SiCnws reinforced CrSi2-SiC/SiC coating was prepared on C/C composites by a two-step pack cementation. Comparative analysis revealed that SiCnws-reinforced coating exhibited better densification with lesser cracks and pores. Isothermal oxidation tests at 1773 K in static air demonstrated exceptional performance: the SiCnws-reinforced coating showed only 14.98% mass loss after 30 h, while the unreinforced coating suffered 36.53% mass loss after 14 h. XRD/SEM characterization confirmed that SiCnws enhanced structural integrity by promoting the formation of a continuous SiO2-Cr2O3 glassy layer during oxidation, while mitigating crack propagation through pinning and bridging effects.
研究领域:
材料科学
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陶瓷涂层
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高温氧化
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纳米材料
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复合材料
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Zupeng Chen,Yongqi Zhuang,Yuguo Dong,Yanmei Zheng,Wenjun Zhang,Lin Dong
Lignin, the most abundant natural aromatic polymer on Earth, offers a promising feedstock for the production of value-added aromatic products through selective C-C bond cleavage. However, achieving both high product yield and selectivity under mild conditions, such as under visible-light irradiation, remains a significant challenge. In this study, we address this issue by employing ceria (CeO2) as a support to precisely engineer the dispersion of vanadium oxide through two distinct catalyst pretreatment methods: impregnation–calcination (Im-V/CeO2) and physical mixing–calcination (Pm-V/CeO2). The results demonstrate that the Im-V/CeO2 catalyst exhibits superior performance, converting 1,2-diphenylethanol to benzaldehyde with an impressive 89% yield and 98% selectivity, while CeO2 alone yields 52% and Pm-V/CeO2 yields 45%. This enhanced performance of Im-V/CeO2 is attributed to the introduction of low-polymerized vanadium oxide (VOx) species. Unlike highly polymeric V2O5 crystals, these species facilitate the separation of photogenerated electron-hole pairs and reduce charge transfer resistance, thereby improving photocatalytic efficiency. Additionally, the polar nature of VOx species enhances the activation of lattice oxygen, creating more sites for oxygen adsorption and activation. In-depth mechanistic studies reveal that superoxide radicals play a dominant role in the C-C bond cleavage process. This innovative strategy for achieving high-efficiency photocatalytic C-C bond cleavage through the controlled dispersion of vanadium oxide on a cerium oxide support offers valuable insights for the sustainable valorization of lignin.
研究领域:
催化
·
材料科学
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光催化
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可持续化学
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木质素高值化
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