ENERGY & FUELS
·
2026
·Vol. 40
·期 30
·16618-16630
·
IF 6
Zhang Jing,Liu Fang-Jing,Xia Lei,Wang Meng-Jie,Xia Wei-Zhen,Zhao Mei-Xia,Zhao Yun-Peng,Zhong Mei,Wei Xian-Yong
Selective cleavage of stable C–C bridging bonds
in the macromolecular
framework of low-rank coal is crucial for its mild conversion to aromatics.
Herein, a bifunctional CoMoS/HY catalyst, featuring highly dispersed
CoMoS nanosheets anchored on ordered HY channels (3–4 nm),
was successfully constructed for the selective hydrocracking of low-rank
coal. Strong metal–support interactions stabilize surface Mo
species and enrich weak acid sites. The weak Lewis acid sites are
primarily responsible for driving the polarization and activation
of C–C bridging bonds. Consequently, the incorporation of HY
remarkably boosts intrinsic activity, giving outstanding turnover
frequencies (TOF) of 85.4 h –1 for Mo and 89.7 h –1 for acid sites (both three times higher than unsupported
CoMoS). Under mild conditions (270 ° C, 2 MPa H 2 , 3
h), the catalyst achieved 98.70% diphenylmethane conversion with >96%
selectivity for arenes. When applied to catalytic hydrocracking of
residue from the thermal dissolution of Naomaohu coal, it produced
a liquid oil yield of 37.2 wt %, which is more than five times higher
than that of the noncatalytic hydrocracking, while also demonstrating
deoxygenation and coke suppression capabilities. This work highlights
a metal–acid-driven synergistic pathway for the efficient conversion
of low-rank coal into high-value arenes.
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ACS Catalysis
·
2020
·
IF 12.35
Peng Zhou,Yuguang Chao,Fan Lv,Kai Wang,Weiyu Zhang,Jinhui Zhou,Hui Chen,Liang Wang,Yiju Li,Qinghua Zhang,Lin Gu,Shaojun Guo
Photocatalytic reforming of renewable and low-cost biomass is an alternative approach to synthesize high-value-added multicarbon compounds and hydrogen. However, the difficulty in activating the methyl group of biomass and simultaneously promoting the C–C coupling makes photocatalytic reforming still a great challenge. Herein, through the first-principles simulation calculation of the energy barrier of acetone dehydrogenation and conversion over a series of noble metal single atom (Ru, Rh, Pd, Ag, Os, Ir, Pt, and Au)-loaded TiO2 (MSA-TiO2) photocatalysts, we predict a Pt single atom-loaded TiO2 (PtSA-TiO2) photocatalyst that can enable methyl activation, CH3COCH2• radical formation, and hydrogen production most effectively from acetone, which is very significant for the synthesis of high-value-added multicarbon compounds by C–C coupling. This is well confirmed by our photocatalytic experiments, revealing that PtSA-loaded commercial P25-TiO2 exhibits the best photocatalytic activity of 3.87 mmol g–1 h–1 for the direct coproduction of high-value-added 2,5-hexanedione (HDN) and hydrogen from acetone with a selectivity of 93%, at least 13-fold higher activity than other noble metal (Ru, Rh, and Ir) single atoms or Pt nanoparticle-loaded ones. In situ attenuated total reflection infrared spectroscopy reveals that the PtSAs contribute to the effective methyl activation and simultaneously promote the formation of more intermediate CH3COCH2• radicals, which are further confirmed by in situ electron spin resonance spectroscopy.
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BIORESOURCE TECHNOLOGY
·
2020
·
IF 7.539
Yong Huang,Shasha Liu,Jie Zhang,Syed Shatir A. Syed-Hassan,Xun Hu,Hongqi Sun,Xun Zhu,Jianbin Zhou,Shu Zhang,Hong Zhang
This study investigated the interactions between volatile and char during biomass pyrolysis at 400 °C, employing a β–5 lignin dimer and amino-modified graphitized carbon nanotube (CNT–NH 2 ) as their models, respectively. The results demonstrated that both –NH 2 and its carrier (CNT) facilitated the conversion of the β–5 dimer, which significantly increased from 9.7% (blank run), to 61.6% (with CNT), and to 96.6% (with CNT–NH 2 ). CNT mainly favored the breakage of C–O bond in the feedstock to produce dimers with a yield of 55.5%, while CNT–NH 2 promoted the cleavage of both C–O and C–C bonds to yield monomers with a yield up to 63.4%. Such significant changes in the pyrolysis behaviors of the β–5 lignin dimer after the introduction of CNT–NH 2 were considered to be mainly caused by hydrogen-bond formations between –NH 2 and the dimeric feedstock/products, in addition to the π–π stacking between CNT and aromatic rings.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2021
·
IF 5.302
Zhenxiao Tang,Maozhong Yi,Qiuling Xiang,Yuhui Du,Ke Peng
An improved high-solid-loading slurry impregnation process was developed to introduce HfB 2 particles into a low-density C/C preform efficiently, and precursor infiltration and pyrolysis process was used for densification to obtain a C/C-HfB 2 -SiC composite. The microstructure characterization revealed that HfB 2 particles uniformly filled the pores in the C/C preform, and SiC well densified the interstices between HfB 2 particles and the small pores in the carbon fiber bundles. After being tested, the C/C-HfB 2 -SiC composite had a density of 4.07 g/cm 3 and a bending strength of 344.8 MPa, and exhibited a non-brittle fracture behavior. After ablation with oxyacetylene flame at 2500 ℃ for 120 s, the mass ablation rate and linear ablation rate of the C/C-HfB 2 -SiC composite were 0.5 mg/s and 0.415 μm/s, respectively. The good ablation performance is attributed to the hindering effect of the HfO 2 scale on oxygen diffusion at high temperature.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Dan Li,Zuquan Gan,Cailin Zhang,Xiuqiu Wang,Mingzhen Zheng,Xiaoyun Gao,Yue Huang,Youjun Fan,Shuifeng Zhang,Fuqin Zheng,Wei Chen
The exploration of sustainable approaches for plastic waste disposal has emerged as an urgent imperative task. This research presents an innovative and eco-friendly electrochemical route to degrade plastic waste, ethylene glycol (EG), into value-added formate. To this end, an interesting hollow FeOOH/CoOOH heterostructure is successfully fabricated for EG oxidation. The difference in work functions between FeOOH and CoOOH results in the establishment of a built-in electric field (BEF), which is beneficial for the adsorption of EG and *OH. As a result, the FeOOH/CoOOH demonstrates outstanding catalytic performance in the EG oxidation reaction (EGOR) with an exceptionally low potential of only 1.32 V at 10 mA cm -2 and a high Faraday efficiency of 92.19% for formate generation. Glycollic acid is identified as a pivotal intermediate in the EGOR by in-situ infrared spectroscopy. Theoretical computations disclose that the FeOOH/CoOOH heterostructure not only causes an upward shift of the d-band center but also largely enhances the *OH adsorption, thus speeding up the cleavage of the inert C-C bond and markedly facilitating the conversion of EG to formate. This research not only enriches the fundamental comprehension of the EGOR but also provides deep insights for the rational design of highly selective and active EGOR catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Sixun Li,Na Wang,Baiqi Hao,Han Li,Qun Xu,Ziqiu Ren
Graphitic nitrogen (N) is the optimal N configuration for peroxymonosulfate (PMS) activation, yet its formation is poorly controllable and usually scarce in N-doped carbon catalysts. Herein, a novel zigzag “N-C-C-S” engineering strategy via sulfur (S)-assisted doping is developed to fabricate S, N co-doped porous carbons (S x N-PCs). Precise tuning of S/N ratio induces N configuration reconstruction, increasing graphitic N content. S 0.57 N-PC affords a 3.1-fold enhancement in PMS activation activity, completely removing bisphenol A (BPA) with a high reaction rate constant (0.597 min -1 ). The “N-C-C-S” moiety enables dynamic switching of reaction mechanisms from radical-initiated degradation to 1 O 2 -mediated mineralization via tailored electronic states of graphitic N. Characterizations and theoretical calculations reveal that S atoms can occupy carbon matrix defects, triggering electron redistribution between adjacent N and C atoms to lower the energy barrier for graphitic N formation. Furthermore, the “N-C-C-S” moiety forms an electron-delocalized system that modulates graphitic N to a moderately electron-enriched state, preserving HSO 5 - adsorption capacity while reducing the energy barrier of PMS decomposition. This optimized electronic state of graphitic N stabilizes active O* intermediates and reduces their formation energy barrier, thereby promoting 1 O 2 generation. A continuous-flow system using S 0.57 N-PC@PVDF membrane demonstrates exceptional durability over 36 h in real-world wastewater treatment.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Wei Hua,Xiya Yang,Zhangyi Zheng,Mutian Ma,Kun Feng,Daqi Song,Peng Liu,Fenglei Lyu,Jun Zhong,Zhao Deng,Yang Peng
Electrocatalytic CO 2 reduction (eCO 2 R) in acidic electrolytes is propitious to enhance CO 2 utilization, yet suffering from low current efficiency due to the rapid kinetics of the competing hydrogen evolution reaction (HER), especially under high current densities. This study proposes the implementation of a single-atom NiNC cocatalyst concurrently generating CO and releasing OH − to neutralize H + in the electrolyte, thereby simultaneously suppressing HER and promoting C–C coupling. By homogeneously mixing the NiNC cocatalyst with Cu nanoparticles (NPs), as opposed to a stratified configuration, a high ethylene Faradaic efficiency (FE) of 57% was achieved at 600 mA cm −2 in acidic media, along with a remarkable single-pass CO 2 conversion efficiency of 52.4%. While rotating disk electrode tests and operando Raman spectroscopy attest to the restricted H + diffusion and elevated local pH near the catalyst surface, in situ Infrared and differential electrochemical mass spectrometries corroborate the spillover of CO from the cocatalyst to neighboring Cu NPs for enhanced C–C coupling. This work offers new insights into the design and application principles of compositional eCO 2 R catalysts for promoting multicarbon synthesis in acidic media at high current density.
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INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Shaochao Sun,Junqiang Zhang,Min Hong,Jialong Wen,Jiliang Ma,Runcang Sun
The utilization of photocatalysis for the simultaneous production of valuable fine chemicals and fuels from biomass-derived feedstocks holds significant promise; however, its practical implementation remains constrained. In this study, we present the development of an Fe-doped gallium nitride (GaN) catalyst treated by calcination (Fe@GaN-X) for the selectively conversion of biomass-based monosaccharides and xylan into lactic acid and carbon monoxide (CO). Fe@GaN-400 exhibited broader visible light absorption, lower resistance, and reduced photoluminescence intensity in comparison to pristine GaN, thereby affording exceptional photocatalytic activity (lactic acid yield: 71.38%; CO evolution rate: 385.74 μmol g −1 h −1 ). When monosaccharides and xylan were used as substrates, the Fe@GaN-400 system demonstrated outstanding photocatalytic activity, particularly in the case of xylan system (CO evolution rate = 923.21 μmol g −1 h −1 ). Additionally, the experimental results revealed the generation of distinctive reactive species, encompassing holes (h + ), superoxide anion (·O 2 - ), hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) within this catalytic system. Remarkably, the ·O 2 - and h + exhibit heightened selectivity towards CO and lactic acid, respectively. This work establishes a novel pathway for the co-production of fine chemicals and fuels through the photocatalytic conversion of biomass.
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CORROSION SCIENCE
·
2019
·
IF 6.355
Haibo Ouyang,Yulei Zhang,Cuiyan Li,Guibiao Li,Jianfeng Huang,Hejun Li
C/C-ZrC-SiC composites were fabricated by carbothermal reaction of hydrothermal co-deposited oxides and resulted in homogeneous microstructure. The fracture behavior passed from pseudo-plastic to brittle fracture with the increase in ZrC/SiC molar ratios. The composites with a molar ratio of ZrC/SiC≈2:1 presented outstanding ablation resistance with a mass ablation rate of 0.06 mg cm −2 s −1 and a linear ablation rate of 0.13 μm s −1 . The optimal ZrC/SiC molar ratio provided a suitable balance of viscosity and flowability of the oxides scale, which not only possessed enough solid ZrO 2 to endure the scouring but also had moderate liquid-phase to seal the defects and limited the oxidation.
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SURFACE & COATINGS TECHNOLOGY
·
2024
·
IF 5.3
Xinzi Zhong,Liyun Cao,Tian Ji,Jianfeng Huang,Yijun Liu,Xuetao Shen,Yong Zhao,Zhiwen Cheng,Ting Liu
Antioxidant SiO 2 coating exhibits low cost and great compatibility with existing uses, but is strongly limited by its poor fluidity and high oxygen permeability from 973 K to 1273 K. Therefore, the hierarchical-design Glass/MoSi 2 -B 2 O 3 @SiO 2 -SiC coating was fabricated on C/C composite by a simple embedding method, and followed by a hot dip process. This composite yielded excellent combination of long-term antioxidant abilities and thermal shock resistances. As oxidized at 973 K for 1500 h, its mass loss was 0.35 %, and only 0.66 % at 1073 K for 2600 h. After thermal shocks 270 times, the weight loss was only 0.56 %. Interestingly, the Glass/MoSi 2 coating acted as a self-healing encapsulation shelter against oxygen, whilst the B 2 O 3 @SiO 2 layer yielded stable healing effect. The B 2 O 3 @SiO 2 microcapsule facilitated the activation of B 2 O 3 , SiO 2 phases, and borosilicate glass sequentially as temperature rose, leveraging their unique advantages in defect healing. Through the synergistic effects of interface encapsulation and defect self-healing, the oxygen kept osmotic diffusion. This study underscores the significance of hierarchical designs in coatings, facilitating structure optimizations and enhancing antioxidant capabilities at multiple levels.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yun Tang,Jingqi Ruan,Yalou Xin,Xiaohu Ren,Hudie Yuan,Xianhu Liu,Qiang Chen
The development of metal–organic frameworks (MOFs)-derived magnetic carbon-based materials for high-efficiency electromagnetic wave (EMW) absorption has attracted widespread attention. While these MOFs-derived composites have shown exceptional performance in absorbing EMWs within the X and Ku bands, the pursuit of effective absorption at lower frequencies remains a challenge. Herein, we demonstrate a novel strategy to synthesize hollow Co@C/C rods with excellent C-band EMW absorption via acetic acid etching and pyrolysis of core–shell ZIF-8@ZIF-67. Based on acetic acid etching, ligand-deficient ZIF-8@ZIF-67 rods with abundant mesoporous structures are constructed, enabling precise control over the Co nanoparticles content, graphitization degree, and pyridinic N doping in the derived Co@C/C. This simple fine-tuning approach simultaneously reduces dipole polarization by lowering the pyridinic N doping concentration, suppresses interfacial polarization and conduction loss through reducing the number of graphitic carbon layer, and enhances magnetic loss by increasing the Co content. These combined effects collectively improve the impedance matching of Co@C/C for low-frequency absorption. Notably, as the volume of acetic acid solution increases, the absorption frequency band of Co@C/C gradually shifts from the Ku-band to the C-band, while sustaining superior EMW absorption performance. At the filling ratio of merely 11 %, the RL min values for Co@C/C-20 and Co@C/C-30 achieve −49.8 dB and −34.7 dB at 7.2 GHz and 6.8 GHz, respectively. This study offers a valuable approach to the development of lightweight materials with excellent EMW absorption in C-band.
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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Yuling Li,Weiran Zhao,Xiang Xiang,YunLei Hu,Xiaoqiang Zhang,Wenjian Sun,Xiaoxuan Liu
Background Perturbed lipid metabolism in cellular environment plays an essential role in the progression of peripheral neuropathy, such as Charcot-Marie-Tooth disease type 1A (CMT1A). Current deep-profiling of lipidome still has certain limitations for high-throughput analysis of clinical samples, such as low sensitivity, extensive requirement of instrument modification, technician-dependent pretreatment and lack of method-adapted data-processing software. Results Herein, a new generation aza-Prilezhaev aziridination (APA) reagent has been designed for coupling with high-resolution liquid chromatography mass spectrometry (LC-MS) to conduct comprehensive untargeted deep lipidomics of CMT1A disease. It facilitates large-scale lipid structural annotations over a wide polarity range in a single run with high-sensitivity. With the developed method, an extensive library containing information on retention time, m / z , and MS/MS down to C=C location levels for 393 unsaturated lipids of CMT1A was created. Significant disease-related differences in C=C isomer profiles were observed from the comparison of plasma between CMT1A patients (N=9) and controls (N=8). Specifically, 40 different lipids were identified, predominantly comprising n-6, n-7, and n-9 C=C positional isomers. Significance This innovative methodology would offer substantial potential to enhance diagnosis and therapeutic strategies for CMT1A and other diseases based on lipid isomerization information.
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