Materials Today Energy
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2026
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IF 8.1
Yipeng Nie,Longquan Deng,Zipei Cui,Zhao Jiang,Wenchao Sheng
Coupling hydrogen evolution reaction (HER) with glycerol oxidation reaction (GOR) in a hybrid electrolyzer represents a highly promising approach for green hydrogen production and glycerol upgrading. However, the limited activity and stability of existing GOR catalysts restrict the energy efficiency of the coupled system. In this study, Pd/C and Pd 4 Ag x /C catalysts were synthesized to investigate the impact of Ag on the activity and stability of Pd-based catalysts for GOR. The optimized Pd 4 Ag 8 /C demonstrated a specific activity of 17.4 ± 0.1 mA cm −2 Pd and a mass activity of 13.2 ± 0.3 A mg −1 Pd , both being more than 10 times higher than those of Pd/C. Combined results of ultra-performance liquid chromatography and density functional theory calculations revealed that the introduction of Ag promotes C−C cleavage in glyceric acid on Pd sites, facilitating electron transfer in GOR and thereby enhancing the GOR activity. The GOR coupled HER hybrid electrolyzer using Pd 4 Ag 8 /C as the GOR catalyst achieved a significant reduction of ∼1.07 V in cell voltage compared to conventional water electrolysis system at a current density of 10 mA cm −2 with a favorable operational stability, and realized the production of high-value-added chemicals, demonstrating the promising potential in both hydrogen production and upgrade of glycerol.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yingying Qian,Houyu Yu,Qihuan He,Dandan Fan,Gerben J. Zylstra,Hancheng Wang,Xing Huang
The extensive application of cyhalofop-butyl, an aryloxyphenoxypropionate (AOPP) herbicide, for weed control in rice fields inevitably results in environmental pollution and ecological toxicity. Microbial degradation of cyhalofop-butyl is garnering immense research attention. This study revealed that Sphingobium yanoikuyae B1 can efficiently degrade the cyhalofop-butyl, completely breaking down 30 mg/L within 12 h via ester bond hydrolysis, forming cyhalofop acid. A novel hydrolase gene cbeH (37.39% identity) was identified in B1. CbeH exhibited catalytic activity by hydrolyzing the ester bond (C-O) in cyhalofop-butyl and other AOPP herbicides, yielding AOPP acids. Additionally, it catalyzed the cleavage of the C-N bond in amide herbicides propanil and diuron, as well as the C-C bond in the aromatic compound 2-hydroxy-6-oxo-6-phenylhexa-2,4-dienoic acid. Sequence alignments and site-directed mutagenesis indicated the catalytic triad Ser-His-Asp in CbeH serves as active center cleaving C-O, C-C, and C-N bonds. Comparative analysis revealed the gene cbeH , highly conserved within Sphingomonads , was located within multiple insertion sequences on the plasmid of Rhodococcus strains. CbeH was widespread in Proteobacteria and Actinobacteria, with its host strains prevalent in aromatic-polluted environments. This study provides novel enzyme resources for remediating combined pollution and enhances our understanding of the genetic organization and environmental distribution of trifunctional pollutant-degrading genes.
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GREEN CHEMISTRY
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2025
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IF 9.2
Shilei Zhang,Hang Wang,Yang Wang,Min Zhang,Weimin Wang,Liang Zhang,Jun Li,Xun Zhu,Qian Fu,Qiang Liao
Elevating the operating pressure could significantly enhance CO2 accessibility on the catalyst in electrochemical CO2 reduction (CO2RR); however, achieving selective production of multi-carbon (C2+) products under pressurized conditions remains a critical challenge because elevated pressure could shift the selectivity towards C1 products. This work systemically investigated the variation of product selectivity induced by pressure and electrolyte composition, and demonstrates that a local pH drop induced by increased pressure is the key reason for hindered C–C coupling, as confirmed by in situ Raman and multi-physics simulation. The elevated pressure results in an increase of the electrolyte's buffering capacity, which neutralizes the alkaline microenvironment near the catalyst, thereby impeding the C–C coupling. Decreasing the buffering ability (using non-buffered KCl electrolyte) or increasing the current density (from 0.4 A cm−2 to 1.0 A cm−2) could maintain a high interfacial alkalinity under elevated pressure, promoting C–C coupling. By mapping pressure–current density operational windows, the optimal conditions were identified, achieving 70% C2 faradaic efficiency (50% for C2H4) at 5 bar and 1 A cm−2, demonstrating superior C2 product selectivity. This work establishes electrolyte engineering principles for industrial CO2RR, enabling carbon-neutral chemical production under practical pressurized conditions through microenvironmental regulation.
研究领域:
电化学
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催化
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材料科学
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化学工程
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环境科学
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GREEN CHEMISTRY
·
2026
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IF 10.6
Yuguo Dong,Puyan Bai,Hongyu Yang,Lin Dong,Xiaoli Gu,Changle Zhao,Zupeng Chen
Photocatalytic depolymerization of lignin into aromatic compounds is of great significance but extremely challenging, hindered by the stable interunit C-C bonds with high dissociation energies. Herein, we develop a novel oxidation acetalization strategy for the phtocatalytic cleavage of C-C bond in lignin model compounds while simultaneously reducing aldehyde condensation. Phosphorus-doped carbon nitride (Px-CN) was synthesized for the selective cleavage of Cα-Cβ bonds under visible light at room temperature. This approach achieves a nearly complete conversion (>99.9%) of 2-phenoxy-1phenylethanol, along with high yields of benzaldehyde dimethyl acetal (91.1%) and benzyl formate (56.3%). Mechanistic investigations reveal that the activation of the Cβ-H bond by photogenerated holes is crucial for the transformation to occur.Meanwhile, the introduction of phosphorus accelerates the separation efficiency of charge carriers, thereby enhancing the photocatalytic performance of the Px-CN. This work demonstrates the potential of phosphorus-doped carbon nitride for the high-selectivity photocatalytic cleavage of the C-C bond in lignin to aromatic chemicals.
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Catalysis Science & Technology
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2026
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IF 4
Yuzhen Hu,Ruiying Xiong,Xin Qu,Taras Nagornyy,Zhenlong Song,Xingye Zeng,Ning Li,Qi Zhang,Longlong Ma
Selective C-C bond cleavage in lignin is a pivotal step toward its efficient utilization, enabling the production of diverse and valuable chemicals from this abundant and renewable resource. Among the catalysts reported for oxidative cleavage of C-C bond in lignin β-O-4 ketones, CeO₂-supported Pd catalysts have demonstrated outstanding activity. However, the exact nature of the active Pd sites responsible for C-C bond cleavage remains poorly understood, limiting mechanistic insights into this transformation. In this study, CeO₂ supports with four distinct morphologies including rods (R), spheres (S), cubes (C), and polyhedrons (P) were synthesized to investigate their influence on the catalytic activity of Pd/CeO₂ catalysts in the oxidative cleavage of β-O-4 ketones. The catalytic performance was found to depend strongly on the morphology of CeO₂, with Pd/CeO₂-P exhibiting the highest activity for C-C bond cleavage. This catalyst possessed the lowest Pd⁴⁺ content and the highest Pd⁰/Pd²⁺ ratio among the series. By systematically tuning this ratio, a volcano-type relationship between Pd⁰/Pd²⁺ ratio and catalytic activity was established, indicating a dual-site mechanism in which Pd⁰ facilitates the formation of reactive oxygen species, while Pd²⁺ serves as the active center for C-C bond cleavage.
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ANALYTICAL CHEMISTRY
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2026
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IF 7.3
Yuanxia Lv,Zhihao Zhao,Shijiao Chen,Ru Ma,Ziqin Lu,Zhimin Zhang,Qian Wu,Hongmei Lu
Spatially resolved profiling of lipid carbon–carbon double bond (C═C) isomers, especially for poorly ionizable glycosphingolipids, remains a significant challenge in mass spectrometry imaging (MSI). Herein, we report a novel MSI method that leverages a diselenide-functionalized covalent organic framework (COF–Se2) by integrating its heterogeneous catalysis and selective surface capture capabilities for on-tissue lipid capture-epoxidation, enabling the differentiation of C═C position isomers with significantly enhanced coverage for glycosphingolipids. In a finely tuned solvent environment, neutral glycosphingolipids were selectively captured and catalytically epoxidized on the COF–Se2 surface with near-quantitative efficiency (∼100%), thereby achieving their separation from epoxidized phospholipids and largely reducing ion suppression. The subsequent desorption of epoxidized glycosphingolipids for mass spectrometry (MS) analysis was allowed by switching the solvent to ammonia-methanol. Epoxidized lipids generate diagnostic fragments for the C═C position in MS/MS, with glycosphingolipids showing distinct patterns from the reported phospholipids and fatty acids. By coating COF–Se2 onto slides for tissue thaw-mounting, on-tissue capture-epoxidation was completed within 5 min. With a two-step ambient liquid extraction MS/MS imaging workflow, epoxidized phospholipids and glycosphingolipids on tissue were imaged separately in each step. Compared with the conventional method, this strategy substantially improved the lipid coverage of isomer-differentiated MSI by 7-fold in brain tissue, especially for glycolipids or sphingolipids (27 vs 0). This work illuminates the inaccessible spatial landscape of glycosphingolipid C═C isomers, opening new avenues for understanding their roles in brain function and disease.
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ACS Catalysis
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2026
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IF 13.6
Du Ruiqi,Guo Na,Zhang Yinan,Chen Zemao,He Junliang,Zhang Chun,Cheng Yi
The oxidative cleavage of C–C bonds is a key reaction pathway in the electrocatalytic valorization of biomass-derived alcohols. However, the influence of molecular branching on this process remains poorly understood. Herein, we establish a nucleophilic hydroxide-mediated C–C cleavage mechanism on Ni(OH) 2 catalyst using isobutanol as a model β-branched primary alcohol. Combining 18 O isotope labeling with in situ mass spectrometry, we demonstrate that isobutyraldehyde is the key intermediate and that hydroxide anions (OH – ), rather than surface-adsorbed *OH, act as the active species driving C–C cleavage. Density functional theory (DFT) studies reveal that the β-branching creates steric hindrance that suppresses C–H dehydrogenation while simultaneously strengthening the van der Waals adsorption of the isobutyraldehyde intermediate. This enhanced adsorption lowers the energy barrier for nucleophilic attack by OH – . This work establishes a fundamental structure–reactivity relationship, offering a strategic blueprint for modulating reaction pathways in biomass upgrading.
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Applied Materials Today
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2023
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IF 8.3
Guiyang Yu,Ke Gong,Lan Hu,Chuanwang Xing,Yujia Hu,Debao Wang,Xiyou Li
The development of mild and environmental method for direct transformation of aromatic alcohol into hydrobenzoin via controlled C‒C coupling is a highly attractive but challenging goal. In this paper, a P-doped g-C 3 N 4 photocatalyst with NiS nanoparticles modification is first reported to apply the visible-light-driven C‒C coupling of aromatic alcohol into hydrobenzoin, as well as integrating with the production of clean H 2 fuel. The synergistic effect of doped P atoms and formed type-II heterojunction between PCN and NiS improves the light absorption ability of g-C 3 N 4 and greatly suppresses the charge recombination. Optimized 2.0% NiS/PCN composite achieves the complete conversion of aromatic alcohol within 6 h reaction time, as far as we known, which is the highest efficiency so far for aromatic alcohol conversion via photocatalytic strategy. Hydrobenzoin is controllably formed with 68% selectivity, together with a highly-efficient H 2 production rate of 994.8 μmol·g −1 ·h −1 . In-situ EPR studies reveal a preferential activation of C‒H bond than O‒H bond in aromatic alcohol by photoexcited holes, forming C 6 H 5 ĊH 2 OH radicals for subsequent coupling. The residual protons interact with photoexcited electrons to generate H 2 . Our study not only offers an efficient g-C 3 N 4 -based photocatalyst for the synthesis of hydrobenzoin under mild conditions, but also opens up a new avenue for manipulating the activation of C‒H or O‒H bonds for high selectivity of hydrobenzoin product.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Junjie Xu,Wei Sun,Xiang Xiong,Hongbo Zhang,Lingkun Yang
To improve the mechanical properties and ablation resistance of Cf-reinforced ceramic-based materials, ZrC–W cermet composites (C/C–ZrC–W) were prepared in C/C preforms using slurries and low-temperature reactive melt infiltration , and their microstructure, formation mechanism, and mechanical and ablation properties were investigated. The obtained results revealed that the formation of C/C–ZrC–W composites involved the dissolution–precipitation and C diffusion processes. Owing to the precipitation of W nanoparticles in the ZrC phase and interdiffusion of W/ZrC, the fabricated C/C–ZrC–W composites exhibited superior mechanical properties with a flexural strength of 280.65 ± 12.84 MPa and fracture toughness of 13.87 ± 0.56 Mpa.m 1/2 . The formation of a Zr–W–O dense oxide layer resulted in the excellent ablation performance of the C/C–ZrC–W composites in oxyacetylene flame with a temperature of 2200 °C, and their mass ablation rate and linear ablation rate were 1.14 mg/s and 2.42 µm/s, respectively. The described method can be potentially used for preparing high-strength, high-toughness, and ablation-resistant materials at low temperatures.
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CERAMICS INTERNATIONAL
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2023
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IF 5.2
Junjie Yan,Xiumei Wu,Qidong Liu,Yunping Li,Shu Yu
Silicon oxycarbide (SiOC) coatings were prepared through isothermal chemical vapor co-deposition by using two precursors of hexamethyldisilane (HMDS) and tetraethyl orthosilicate (TEOS). The microstructure, composition and the protectiveness on C/C composite against oxidation of the coatings prepared at temperatures ranging from 1423 K to 1563 K and pressures ranging from 500 Pa to 1200 Pa were investigated, respectively. After oxidation, cracks and defects were formed in the coatings of all conditions due to the volume shrinkage of amorphous SiO 2 crystallization and the mismatch of thermal expansion coefficient (CTE) between SiOC coatings and substrate. The most oxidation-resistant SiOC coating was obtained at 1563 K and 500 Pa, which exhibited the lowest weight loss rate of 4.87 % after 12 h of oxidation at 1673 K in air condition.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Jiayuan Sun,Shanshan Shao,Xinggang Hu,Xiaohua Li,Huiyan Zhang
The aqueous fraction of bio-oil from biomass fast pyrolysis mainly contains low-molecular-weight oxygenates such as carboxylic acids, ketones, aldehydes, phenols, and furans. In this study, the full components of aqueous bio-oil are directionally converted into carbonyl groups such as aldehydes and ketones, and then the oxygen-containing precursors of aviation fuel are prepared through coupling, focusing on exploring the mechanism of carbonylation and C–C coupling. Studies have revealed that propionic acid, furfural, and phenol can be directionally converted into ketones, in which reaction 3-pentanone, cyclopentanone, and cyclohexanone were formed via ketonization and hydrogenation in the aqueous phase. Then the two components of 3-pentanone, cyclopentanone, cyclohexanone, acetone, and acetaldehyde were subjected to aldol condensation to explore the C–C coupling mechanism in the preparation of the C7–C18 precursor of aviation fuel. The mechanism in the high-quality utilization of all components of the aqueous phase bio-oil fraction was explored, which was favorable for the synthesis of biomass-based aviation fuel.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Yingying Zhou,Jia-jia Jiao,Huang Huang,Yong Dong Liu,Rugang Zhong,Xin Yang
Dichloroacetonitrile (DCAN) as one of the potentially prioritized regulated DBPs has drawn great attention; however, understanding its formation, especially the C–C bond cleavage mechanisms, is limited. In this study, DCAN formation mechanisms from long-chain primary amines, amino acids, and dipeptides during chlorination were investigated by a combined computational and experimental approach. The results indicate that nitriles initially generate for all of the above precursors, then they undergo β-C-hydroxylation or/and α-C-chlorination processes, and finally, DCAN is produced through the Cα–Cβ bond cleavage. For the first time, the underlying mechanism of the C–C bond cleavage was unraveled to be electron transfer from the O– anion into its attached C atom in the chlorinated nitriles, leading to the strongly polarized Cα–Cβ bond heterocleavage and DCAN– formation. Moreover, DCAN molar yields of precursors studied in the present work were found to be determined by their groups at the γ-site of the amino group, where the carbonyl group including −CO2–, −COR, and −CONHR, the aromatic group, and the −OH group can all dramatically facilitate DCAN formation by skipping over or promoting the time-consuming β-C-hydroxylation process and featuring relatively lower activation free energies in the C–C bond cleavage. Importantly, 4-amino-2-hydroxybutyric acid was revealed to possess the highest DCAN yield among all the known aliphatic long-chain precursors to date during chlorination. Additionally, enonitriles, (chloro-)isocyanates, and nitriles can be generated during DCAN formation and should be of concern due to their high toxicities.
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