LANGMUIR
·
2024
·
IF 3.7
Mian Gong,Yihui Dong,Minghai Zhu,Fengxiang Qin,Tianchi Wang,Faiz Ullah Shah,Rong An
Surface-enhanced Raman scattering (SERS) is a remarkably powerful analytical technique enabling trace-level detection of biological molecules. The interaction of a probe molecule with the SERS substrate shows important distinctions in the SERS spectra, providing inherent fingerprint information on the probe molecule. Herein, nonhalogenated phosphonium-based ionic liquids (ILs) containing cations with varying chain lengths were used as trace additives to amplify the interaction between the cytochrome c (Cyt c) and Zr–Al–Co–O (ZACO) nanotube arrays, strengthening the SERS signals. An increased enhancement factor (EF) by 2.5–41.2 times compared with the system without ILs was achieved. The improvement of the SERS sensitivity with the introduction of these ILs is strongly dependent on the cation chain length, in which the increasing magnitude of EF is more pronounced in the system with a longer alkyl chain length on the cation. Comparing the interaction forces measured by Cyt c-grafted atomic force microscopy (AFM) probes on ZACO substrates with those predicted by the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) theory, the van der Waals forces became increasingly dominant as the chain length of the cations increased, associated with stronger Cyt c–ZACO XDLVO interaction forces. The major contributing component, van der Waals force, stems from the longer cation chains of the IL, which act as a bridge to connect Cyt c and the ZACO substrate, promoting the anchoring of the Cyt c molecules onto the substrate, thereby benefiting SERS enhancement.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Wenjing Kong,Xueyun Zhong,Ying Yan,Yun Xing,Lei Liu,Chuan Yu,Leneng Yang,Xiaofei Song,Mingli Fu
With the widespread use of waterborne coatings, the treatment of volatile organic compounds (VOCs), which is also easy to produce odor pollution, has become the major concern of the air pollution control in coating industry. Since the deep oxidation of the butyl acetate (BA) molecule requires the involvement of a large amount of reactive oxygen species, the catalytic oxidation of BA was promoted by weakening the Co-O bond strength on the cobalt oxide surface. In this study, we adopted a simple sacrificial template approach to fabricate a series of specifically shaped and uniform Co3O4 catalysts for the catalytic oxidation of BA. The flake CM71-C catalyst showed the most excellent catalytic properties of BA (T50 = 197 °C, T90 = 215 °C). According to the characterization results, flake CM71-C has the largest specific surface area and the weakest Co-O bond, which is more conducive to redox and oxygen activation capabilities of catalyst. The results of In-situ DRIFTS studies showed that the surface reactive oxygen species were continuously recharged during the reaction due to the higher oxygen activation capacity, which accelerated the rapid decomposition of carboxylate, a key reactive intermediate species in the deep oxidation of BA. This study provides a practical and effective way to gain insight into the role of oxygen vacancies in the preparation of efficient catalysts with specific morphology for VOCs oxidation.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
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IF 7.7
Ziwen Yao,Jing Li,Shuai Nie,Yuan Wang,Xitao Yin,Yunxia He
Utilizing p-n composite materials for the fabrication of metal-oxide semiconductor (MOS) gas sensors represents a promising strategy to achieve exceptional selectivity in detecting reducing gases such as hydrogen (H₂) and carbon monoxide (CO). However, previous studies have typically achieved this selectivity under fixed operating temperatures and single molar ratios. This study presents the successful synthesis of n-In₂O₃/p-Co₃O₄ nanoparticles, featuring a p-n heterojunction structure, using a simple composite preparation method. The gas-sensing properties, crystal structure, morphology, and chemical states were comprehensively characterized using an electrochemical workstation, XRD, TEM, HRTEM, and XPS. Experimental results show that the gas sensor responses of the n-In₂O₃/p-xCo₃O₄ composites (with x = 10.5, 15, 18, 21), annealed at 500°C within an operational temperature range of 350°C to 400°C, exhibit distinct behaviors for CO and H₂ gases. This addresses the challenge of achieving selective detection across varying conditions. Notably, the n-In₂O₃/p-18Co₃O₄ composites display opposing response characteristics for both gases across a broad temperature range of 200°C to 400°C. At 350°C, the n-In₂O₃/p-18Co₃O₄ sensor demonstrates optimal selectivity, significantly minimizing cross-sensitivity and improving detection accuracy and reliability. The sensor also shows excellent stability, with consistent responses under repetitive exposure conditions. By improving both sensor selectivity and stability, this research advances gas detection technologies, with potential applications in sustainable energy and public health monitoring.
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Small
·
2024
·Vol. 20
·期 29
·2310087
·
IF 13
Yunfeng Qiu,Yongxia Zhang,Miao Yu,Xinyi Li,Yanxia Wang,Zhuo Ma,Shaoqin Liu
Simultaneously improving electrochemical activity and stability is a long-term goal for water splitting. Herein, hierarchical N-doped carbon nanotubes on carbon nanowires derived from PPy are grown on carbon cloth, serving as a support for NiCo oxides/sulfides. The hierarchical electrodes annealed in N 2 or H 2 /N 2 display improved intrinsic activity and stability for hydrogen evolution reaction (HER) and glucose oxidation reaction. Compared with Pt/C||Ir/C in alkaline media, the glucose electrolysis assembled with electrodes exhibits a cell voltage of 1.38 V at 10 mA cm −2 , durability for >12 h at 50 mA cm −2 , and resistance to glucose/gluconic acid poisoning. In addition, electrocatalysts can also be applied in ethanol oxidation reactions. Systematic characterizations reveal the strong interactions between NiCo and N-doped carbon support-induced partial charge transfer at the interface and regulate the local electronic structure of active sites. Density functional theory calculations demonstrate that the synergistic effect between N-doped carbon supports, metallic NiCo, and NiCo oxides/sulfides optimize the adsorption energy of H 2 O and the H* free energy for HER. The energy barrier of the dehydrogenation of glucose effectively decreased. This work will attract attention to the role of metal-support interactions in enhancing the intrinsic activity and stability of electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Bolong Zhao,Yuyu Wang,Min Xu,Duoning Zhao,Li Zhu,Liqiong Wang,Wenxin Ji,Yuanyuan Li,Guangsuo Yu,Yulong Ma,Yonggang Sun
Low-nuclearity cobalt-oxygen/nitrogen heterogeneous clusters (Co-O/N HCs) activated H 2 O 2 for non-radical oxidation of organic pollutants via unique oxygen atom transfer (OAT) and singlet oxygen ( 1 O 2 ) pathways. The novel Co-O/N HCs were synthesized using a ligand self-polymerization strategy. When applied to high-salinity wastewater, they efficiently degraded tetracycline via 100 % non-radical pathways over a wide pH range, with degradation rates greater than 0.1758 min −1 and no inhibition by Cl - . The confined cluster size (3–5 Co atomic units) and asymmetric nitrogen distribution modified the cobalt atoms' electronic structure, promoting two H 2 O 2 adsorption modes: bridge-adsorbed *O-O* mediated direct oxidation via OAT, while edge-adsorbed *OOH species selectively generated 1 O 2 . This work elucidates the active sites and mechanisms of H 2 O 2 activation, offering key insights for the design of advanced Fenton-like catalysts.
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Small
·
2025
·
IF 12.1
Jiajie Xu,Tenghui Jin,Wei Qu,Kaizhou Huang,Zhiyu Liu,Ping Zhang,Jiaping Paul Chen
Development of high-performance photocatalysts for persulfate activation is often limited by rapid electron–hole recombination and insufficient quantum efficiency. To overcome the challenges, electronic metal–support interaction (EMSI) structure is designed. The innovative structure has several key benefits: recombination rates are significantly reduced, charge separation is enhanced, and content of active sites and intrinsic catalytic activity are increased. ZrO 2 /Co 3 O 4 bimetallic oxides featuring a synergistic Co─O─Zr EMSI coordination are synthesized via a sol-gel method. Strong EMSI effects markedly modulate and stabilize the Co 3d electronic structure, creating an electron-rich center on Co sites to promote persulfate activation, and an electron-deficient center on Zr sites to adsorb atrazine. The Gibbs free energy analysis reveals that Zr incorporation reduces the overpotential of oxygen evolution reaction, thereby facilitating electron transfer, promoting hole consumption and suppressing charge recombination. More importantly, it promotes the generation of reactive oxygen species—predominantly via a singlet oxygen ( 1 O 2 )-dominated non-radical mechanism. The optimized catalyst achieves 97.3% degradation of atrazine (a model compound) under visible light, outperforming commercial catalysts (e.g., 4.5-fold of Co 3 O 4 ). The work elucidates the cooperative mechanism of dual-site engineering and EMSI-mediated electron redistribution, providing a rational strategy for designing efficient photocatalysts toward sustainable advanced oxidation processes.
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ACS Catalysis
·
2024
·
IF 11.3
Baoxin Ge,Pengyang Jiang,Biyi Chen,Caijin Huang
The orbital hybridization between metal and oxygen of perovskite catalysts can lower the overpotential and enhance the oxygen evolution reaction (OER) activity. This study combines density functional theory with experiments to clarify how Sr/Fe codoping modulates orbital hybridization and enhances OER catalytic activity of LaCoO3. The as-prepared La0.50Sr0.50Co0.75Fe0.25O3 shows remarkable performance with a low overpotential of 310 mV at 10 mA cm–2 current density and a 107.03 mV dec–1 Tafel slope, outperforming most state-of-the-art perovskite-based OER electrocatalysts. The experimental results confirm that Sr/Fe codoping enhances the expansion of Co–O–Co bond angles and strengthens the covalency of the Co–O bond in LaCoO3, leading to enhanced electrocatalytic activity. Moreover, increasing Sr doping reduces the distance between the Co 3d/O 2p center and the Fermi level, decreasing the energy difference between them and enhancing the degree of orbital hybridization between Co 3d and O 2p. As the degree of Co 3d/O 2p orbital hybridization increases, a higher charge transfer was found between the active center and intermediate product, OOH, reducing the energy barrier of the rate-determining step while lowering the overpotential. This study provides thorough insight into the rational design of OER catalysts based on orbital hybridization.
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JOURNAL OF THE ENERGY INSTITUTE
·
2026
·
IF 6.5
Yanni Liu,Dong Shen,Jun Liu,Yuqiong Zhao,Guojie Zhang
Dry reforming of methane (DRM) is a promising route for the simultaneous utilization of CH 4 and CO 2 to produce syngas, yet the development of efficient and stable catalysts for low-temperature DRM remains highly challenging. In this work, a series of Co/CeO 2 catalysts with morphology-controlled ceria supports were prepared to investigate the structure–performance relationship in DRM. Among them, the catalyst supported on CeO 2 nanorods (Co/CeO 2 -R) exhibited the best catalytic activity and stability at 600 °C. Structural characterization suggests that the CeO 2 -R support provides a higher surface area and defect density, which favors Co dispersion and the formation of Co-O-Ce interfacial structures. Raman, XPS, and H 2 -TPR results indicate that Co/CeO 2 -R possesses a higher concentration of oxygen vacancies and stronger interfacial interactions compared with other catalysts. CO 2 -TPD measurements further show enhanced CO 2 adsorption capacity, which is consistent with the increased density of defect sites. The results collectively suggest that the improved catalytic performance originates from the synergistic effect of Co dispersion, oxygen vacancies, and Co-O-Ce interfacial structures, which together promote CO 2 activation, oxygen transfer, and carbon removal. In situ DRIFTS results suggest a bifunctional reaction pathway, in which CH 4 activation is likely to occur on Co sites, while CO 2 is activated on defect-rich CeO 2 surfaces to form carbonate/formate species that may participate in carbon removal. Overall, this work establishes a structure-performance correlation between CeO 2 morphology and catalytic behavior, providing insights into the design of Co-based catalysts for low-temperature DRM.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Cong Yuan,Xiaoxiao Zhu,Jiaqi Pan,Minghao Xu,Yongjun Jiang,Sheng Dai,Yikai Huang,Leixi Lu,Lei Zhou,Chengcheng Tian
The understanding of how single atoms anchoring on oxides contribute to high-activity catalysis in the sulfate radical-advanced oxidation process (SR-AOP) remains obscure. Here we presented a new strategy for regulating singlet oxygen ( 1 O 2 ) generation in peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) by engineering the Co-O-X active sites on oxide supports in this study. The Co single atoms supported on mesoporous oxides (Co SA -XO 2 ) were first successfully developed using a modified sol–gel solvent vaporization self-assembly method. We found that Co SA -XO 2 catalysts served as efficient PMS activators for pollutant decomposition over a wide pH range. Notably, Co SA -TiO 2 exhibited exceptional performance, achieving nearly 100% removal of sulfasalazine (SSZ) within 10 min. Furthermore, evidenced by experimental results and density functional theory (DFT) calculations, 1 O 2 was confirmed to be predominately active oxidizing species by the unique Co-O-X bonds for activating PMS in Co SA -XO 2 /PMS system, resulting in an excellent pollution degradation. This study provides valuable insights into the construction of highly loaded single-atom catalysts using oxide substrates in the PMS-AOP system, along with the mechanism of regulating reactive oxygen species (ROS) formation through interfacial bonding between active metal and support.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Zhouzhou Wang,Qiancheng Zhou,Li Luo,Yaran Shi,Haoran Li,Chunchun Wang,Kesheng Lin,Chengsi Wang,Libing Zhu,Linyun Han,Zhuo Xing,Ying Yu
Neutral oxygen evolution reaction (OER) is a crucial half-reaction for electrocatalytic chemical production under mild condition, but with limited development due to low activity and poor stability. Herein, a tungsten-doped cobalt molybdate (WDCMO) catalyst was synthesized for efficient and durable OER under neutral electrolyte. It is demonstrated that catalyst reconstruction is suppressed by W doping, which stabilizes the Co-O-Mo point-to-point connection in CoMoO 4 architecture and stimulates to a lower valence state of active sites over the surface phase. Thereby, the surface structure maintains to avoid compound dissolution caused by over-oxidation during OER. Meanwhile, the WDCMO catalyst promotes charge transfer and optimizes *OH intermediate adsorption, which improves reaction kinetics and intrinsic activity. Consequently, the WDCMO electrode exhibits an overpotential of 302 mV at 10 mA cm –2 in neutral electrolyte with an improvement of 182 mV compared with CoMoO 4 electrode. Furthermore, W doping significantly improves the electrode stability from 50 h to more than 320 h, with a suppressive potential attenuation from 2.82 to 0.29 mV h –1 . This work will shed new light on designing rational electrocatalysts for neutral OER.
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Engineering
·
2025
·
IF 11.6
Qian Hu,Shanli Wang,Kaixing Fu,Guangpeng Yang,Licong Xu,Wenbin Jiang,Minghua Wu,Wangyang Lu,Xiaomin Zhu,Jinming Luo
The singlet oxygen ( 1 O 2 )-driven nonradical oxidation pathway has shown great promise for the degradation of organic pollutants with high ionization potentials (IPs) in complex water matrices because of its longer half-life and stronger resistance to environmental interference. However, the symmetric configuration of the active sites (e.g., Fe–O–Fe) in heterogeneous catalysts largely restricts the efficacy of 1 O 2 generation during ozone activation. In this study, we constructed an asymmetric Co–O–Fe dual-site in bimetallic metal‒organic frameworks (MOFs) with enhanced electron delocalization to switch the ozone activation pathway from radical-dominant to nonradical-dominant. By combining experimental and theoretical analyses, we revealed that breaking the symmetry of iron sites with Co incorporation optimizes the local electronic structure, thereby facilitating ozone adsorption and reducing the O‒O bond scission energy barrier to produce 1 O 2 . As a result, the constructed asymmetric Co–O–Fe dual-site demonstrates impressive 6.6 and 2.0 fold increases in 1 O 2 selectivity and phenol degradation efficiency, surpassing the performance of the state-of-the-art ozonation catalysts. Furthermore, the Co–O–Fe dual-site/O 3 system could efficiently and stably remove diverse high-IP organic pollutants in complex water matrices, following a positive linear correlation ( R 2 > 0.97) between the kinetic rate constants and theoretical IP values, which further highlights the unique and critical role of 1 O 2 . This work advances the understanding and design of efficient dual-site catalysts for selective 1 O 2 generation and sustainable high-IP pollutant degradation.
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CATALYSIS TODAY
·
2019
·
IF 4.888
Tianyu Gao,Yongxuan Yin,Guanghui Zhu,Qiue Cao,Wenhao Fang
Oxidative transformations of HMF are key routes toward a wide variety of chemicals and biofuels through an environmental friendly process. Co 3 O 4 NPs decorated Mn-Co-O solid solution, donated as Co 3 O 4 /Mn X Co, was prepared by co-precipitation method and used as non-precious metal catalyst for base-free oxidation of HMF to FDCA in the presence of O 2 and water. Comprehensive characterizations such as XRD, H 2 -TPR, O 2 -TPD, XPS, NH 3 /CO 2 -TPD and TEM were used to study materials properties especially the oxygen mobility and acidity-basicity. The effect of Mn/Co molar ratio in catalyst and the reaction conditions were investigated and optimized. In addition, the kinetics of the reaction was monitored to reveal the reaction route and rate-determining step. The variation of Mn/Co molar ratio was found to affect not only HMF conversion but also distribution of products. When the Mn/Co ratio was of 0.2, the Co 3 O 4 /Mn 0.2 Co catalyst showed the optimal catalytic performance (i.e., >99% yield of FDCA obtained under 1 bar O 2 at 140 °C after 24 h) due to the highest content of both Lewis and Brønsted acid sites on the surface, leading to the strongest ability of HMF adsorption and COOH group formation, as well as the enhanced oxygen mobility. This catalyst was shown stable after a minor deactivation (≤8%) during six recycling uses and its activity can be entirely regenerated by calcination in air.
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