ACS Nano
·
2025
·
IF 16
Haijuan Zhang,Hengyue Xu,Jie Chen,Daqin Guan,Zhiwei Hu,Xiaomin Xu,Zezhou Lin,Hainan Sun,Xiao Sun,Jiayi Tang,Chih-Wen Pao,Chien-Te Chen,Wei Zhou,Chunchang Wang,Youmin Guo,Zongping Shao
Lattice oxygen participation mechanism (LOM) can break the conventional adsorption scaling limitations to boost electrocatalysis performance and has been utilized to design promising single-phase oxides that generally show favorable bulk oxygen-ion diffusion capability. In pure-phase materials, bulk oxygen vacancies could act as oxygen-ion diffusion channels, implying rich bulk oxygen vacancies at the interfaces of hybrid-phase composites may further boost LOM. Here, by designing hybrid Co2.5Ru0.5Ox hollow nanotubes with rich two-phase interfaces, we report a phenomenon of interfacial LOM. Such hollow nanotubes (∼10 nm wall thickness), composed of spinel Co3O4-x-rutile RuO2-x interfaces, exhibiting a low overpotential of 430 mV and a long-term stability of 1000 h at 500 mA cm–2 for oxygen-evolving reaction (OER) in near-industrial alkaline solutions (6 M KOH). The constructed anion exchange membrane electrolyzer requires only 1.82 V to achieve a 1 A cm–2. Interfacial Co/Ru atomic interactions trigger Co–O–Ru motifs to undergo self-optimization during OER through oxidizing Co/Ru ions and narrowing bond length to create short synergetic active sites, while interfacial oxygen vacancies act as ion-diffusion pathways. Combined mechanism experiments and computations unravel the exceptional interfacial LOM processes. Additionally, the hollow nanotube structure promotes OH– adsorption, serving as a beneficial driving force for interfacial LOM.
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Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Tianhao Yu,peng gao,Hong Du,ling dong
The oxygen evolution reaction (OER) requires the development of a strong and efficient electrocatalyst due to its slow mechanism and high overpotential. Hence, we assembled POM and NiCo-ZIF-67 to obtain the amorphous hollow core-shell material NiCo-ZIF-67@POM (donated as NiCo-ZIF@POM) with high catalytic activity. NiCo-ZIF@POM (1:3) presents a low overpotential (η≈150 mV@10 mA cm-2), a small Tafel slope (100 mV dec-1), and great stability for OER in 1 M KOH solution. Theoretical calculations indicate that the excellent activity of NiCo-ZIF@POM might be attributed to the charge rearrangement due to the interaction between Co and W. In addition, the low electronegativity of P and the high oxidation state of W in POM could accelerate the rapid OH- transfer and induce the intermediates to adsorb on the Co-O-W bridge bond conformation, which improves the performance of the catalytic OER. This study provides a new idea for the secondary assembly of POM and MOF materials.
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Water
·
2025
·Vol. 17
·期 14
·2161
·
IF 3
Qiliang Xiao,Jun Nan
This study presents the development of a novel Cu–Co–O-codoped graphitic carbon nitride (g-C3N4) catalyst for efficient peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX) in aqueous environments. The synthesized Cu–Co–O-g-C3N4catalyst demonstrated exceptional catalytic performance, achieving 90% SMX removal within 10 min—significantly outperforming pristine g-C3N4(14%) and O-doped g-C3N4(22%)—with a reaction rate constant of 0.63 min−1. The superior activity was attributed to the synergistic effects of Cu-Co bimetallic doping and oxygen incorporation, which enhanced the active sites, stabilized metal ions, and minimized leaching. Mechanistic studies revealed a dual-pathway degradation process: (1) a radical pathway dominated by sulfate radicals (SO4•−) and (2) a non-radical pathway driven by singlet oxygen (1O2), with the latter identified as the dominant species through quenching experiments. The catalyst exhibited broad pH adaptability and optimal performance at neutral to alkaline conditions. Characterization techniques (XRD, FTIR, XPS) confirmed successful doping and revealed that oxygen incorporation modified the electronic structure of g-C3N4, improving charge carrier separation. This work provides a sustainable strategy for antibiotic removal, addressing key challenges in advanced oxidation processes (AOPs), and highlights the potential of multi-heteroatom-doped carbon nitride catalysts for water purification.
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POLYMER DEGRADATION AND STABILITY
·
2024
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IF 6.3
Yingbing Zou,Kui Niu,Fubin Luo,Hongzhou Li
The development of metal oxide flame retardants that are easy to synthesize, efficient, and recyclable would be more beneficial to circular economy. In this work, a porous core-shell Mn 3 CoO x was developed to efficiently reduce heat, smoke as well as hazardous gas during the combustion of epoxy resin (EP). Compared with pure EP, the peak heat release rate (pHRR), total heat release (THR), peak smoke production rate (pSPR), total smoke production (TSP), peak CO production rate (pCOPR), and peak CO 2 production rate (pCO 2 PR) of EP/Mn 3 CoO x are reduced by 47.5 %, 21.5 %, 34.6 %, 17.6 %, 58.6 %, and 55.4 %, respectively. It has been shown that Mn 3 CoO x not only catalyzes the formation of high-quality char layer but also effectively catalyzes the conversion of hazardous gas products into CO 2 . Recovery experiments of Mn 3 CoO x filler in EP composites show that the recovery of Mn 3 CoO x can reach 90.0 %. This work provides insights into the design of efficient metal oxide flame retardants and ideas for the development of recycled flame retardants.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yunhui Xia,Bingyan Liu,Mingyuan Zhang,Guohui Cai,Mengjia Zhang,Jianghui Lin,Ling Li
Co-doped CeO 2 creates synergistic Co-O-Ce interfaces and oxygen vacancies. • Distinct CH 3 OH and CO 2 activation sites alleviate competitive adsorption. • Achieves high DMC yield of 16.5 mmol·g −1 ·h −1 under 2 MPa CO 2 and 140 °C. • Excellent stability demonstrated over five consecutive reaction cycles. • In situ IR confirms cooperative mechanism at Co-O-Ce active centers and O V . The direct conversion of carbon dioxide (CO 2 ) and methanol (CH 3 OH) into dimethyl carbonate (DMC) represents a highly attractive route for sustainable chemical synthesis and carbon utilization. However, when operating without dehydrating agents (typically used to shift the thermodynamic equilibrium), the process faces a fundamental challenge on conventional CeO 2 -based catalysts: the competitive adsorption of CO 2 and CH 3 OH for similar active sites, which ultimately limits reaction efficiency. To address this challenge, an innovative strategy was developed through the design of defect-engineered Co 0.05 Ce 0.95 O 2-δ solid solutions. Comprehensive characterization using Raman spectroscopy, XPS, XANES and EXAFS spectra, and AC-TEM confirmed the successful incorporation of Co into the CeO 2 lattice. The incorporation of Co generated abundant oxygen vacancies (O V ) and unique Co-associated interfacial sites (Co-O-Ce). These sites collectively enhanced the catalyst's acidity and basicity and helped alleviate competitive adsorption. Specifically, Co-O-Ce sites are proposed to favor CH 3 OH adsorption and activation, while O V and adjacent Ce ions facilitate CO 2 adsorption and polarization. This cooperative interaction substantially enhances the reaction efficiency, enabling the catalyst to achieve a high DMC formation rate of 16.5 mmol·g −1 ·h −1 under mild conditions (140 °C, 2 MPa), which surpasses that of most reported CeO 2 -based catalysts under comparable conditions. Moreover, the catalyst exhibited outstanding stability over five consecutive cycles. The reaction mechanism, involving the synergistic function of the Co-O-Ce interface sites, was further validated by in situ infrared spectroscopy. Beyond providing a highly efficient and stable catalyst, this work offers fundamental insights into active site engineering for promoting cooperative activation in CO 2 conversion reactions. Download: Download high-res image (339KB) Download: Download full-size image
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 21
·12712-12720
·
IF 10.7
Tianhao Yu,Peng Gao,Hong Du,Ling Dong
Metal–organic frameworks (MOFs) have recently been reported as promising catalysts for the oxygen evolution reaction (OER). Hence, we chose hydroxyl-rich 2,5-dihydroxyterephthalic acid as the ligand to prepare a novel MIL-100 and wrapped it on the NiCo-ZIF-67 surface to obtain an amorphous hollow material (NiCo-ZIF-67@Fe-MIL-100, denoted as NiCo-ZIF@MIL). The composite material presents a low overpotential (η ≈ 139 mV @ 10 mA cm−2), a small Tafel slope (119 mV dec−1) and great stability for the OER in 1 M KOH solution. Density Functional Theory (DFT) calculations show that the hydroxyl-rich structure, which accelerates OH− transfer and promotes the formation of the Co–O–Fe bridge, effectively reduces the reaction energy barrier (from 2.67 eV for NiCo-ZIF-67 to 2.08 eV for NiCo-ZIF@MIL). This work provides an important reference for the development of double-MOF materials.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
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IF 11.2
Tao Zhao,Dazhong Zhong,Qiang Fang,Xin Zhao,Runxin Du,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
The rational design of metal-organic frameworks (MOFs) provides potential opportunities for improving energy conversion efficiency. However, developing efficient MOF-based electrocatalysts remains highly challenging. Herein, a strategy involving strain engineering is developed to promote the electrocatalytic performance of MOFs by optimizing electronic configuration and improving the active site. As expected, the optimized CoFe–BDC NO 2 exhibits a low overpotential of 292 mV at 10 mA cm –2 and a small Tafel slope of 31.6 mV dec –1 as oxygen evolution reaction (OER) electrocatalyst. Notably, when CoFe–BDC NO 2 is prepared on Nickel foam (NF), the overpotential is only 345 mV at 1 A cm –2 , which ensures efficient water oxidation properties. Integrating CoFe–BDC NO 2 /NF anode in membrane electrode assembly (MEA) for overall water splitting and CO 2 reduction reaction (CO 2 RR) tests, the results show that the cell voltages of CoFe–BDC NO 2 /NF are 3.14 and 3.09 V at 300 mA cm –2 (25 °C), respectively, indicating that MOFs have various practical application prospects. The research of the structure-performance relationship reveals the lattice oxygen oxidation mechanism (LOM) where the Co-O-Fe bond is formed during the OER process by changing the electronic environment and coordination structure of CoFe–BDC NO 2 , and with high valence Co as active center, which provides a deep understanding of the structure design of MOFs and their structural transformation during OER.
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FIBERS AND POLYMERS
·
2013
·Vol. 14
·期 1
·8-15
·
IF 0.912
Xu Feng,Jamal Ruxangul,Ubul Aminam,Shao Weiwei,Abdiryim Tursun
The composites of copolymers of aniline (An) and o -methoxyaniline (OMA) with multi-walled carbon nanotubes, named as copolymers/MWNT, (poly(An-co-OMA)/MWNT) were prepared by solid-state synthesis method at room temperature. The homopolymers/MWNT composites were synthesized for comparison. The structure and morphology of these composites were characterized by FT-IR spectroscopy, UV-Vis absorption spectroscopy, X-ray diffraction (XRD) and TEM. The electrochemical performances of the composites were investigated by galvanostatic charge-discharge, cyclic voltammetry (CV) and cycle life measurements. The results from FT-IR and UV-Vis spectra showed that different molar ratio of [An]/[OMA] in reaction system has great influence on the oxidation degree, conjugation length and doping level of the copolymers in these composites. The presence of MWNT in the composites was confirmed from the characteristic peaks of MWNT in XRD patterns and the enwrapped MWNT in TEM images. The TEM images further indicates that the MWNT uniformly distributed and enwrapped with polymer in the case of composite from molar ratio of [An]/[OMA]=1:1. The results also showed that the morphology, crystallinity and solubility of composites were highly affected by the incorporation of OMA unit copolymer chain. The results from electrochemical performances suggested that the molar ratio of [An]/[OMA]=3:1 in reaction system can make the obtained composites displayed a higher specific capacitance, good rate ability and cycling stability.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jili Yuan,Hao Yin,Xin Ge,Ronglan Pan,Caijuan Huang,Dechao Chen,Lin Hu,Haibo Xie
The coordination environment of transition metals in single-atom catalysts (SACs) is crucial for tuning the pathway of the electrocatalytic oxygen reduction reaction (ORR). However, it is significantly difficult to simultaneously and precisely control the first and second coordination structure near the metal active center. Herein, we report that the activated carbon black was used to anchor transition metals’ single atoms with a similar first and second coordination structure. As a result, Co-SACs exhibit an extraordinary performance for ORR to produce H 2 O 2 , where a current density of around ∼2.8 mA cm −2 at 0.1 V vs RHE by rotating ring-disk electrodes and a high yield rate of 110.2 mmol g metal −1 h −1 at the potential of 0.3 V vs RHE in a gas diffusion electrodes (GDEs) cell, with a high positive onset potential of 0.65 V vs RHE and a >80% selectivity of H 2 O 2 at the potential range from 0.25 to 0.65 V vs RHE, respectively. The combined experimental observations and theoretical calculations indicate that the catalytic active center lies in the Co-C 3 /O 1 moiety of the adjacent epoxy group. The possible position of the epoxy group in the second coordination sphere was further revealed. Moreover, Co-SACs were employed in an electrocatalytic GDEs cell for distributed generation of H 2 O 2 in the acidic media, and coupling Fe-SACs-based Fenton filter or electro-Fenton setup with the H 2 O 2 electrolytic generator delivers an efficient and distributable wastewater treatment system. Our study provides a promising and alternative route for on-site H 2 O 2 production coupling the practical application process.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Dengyu Fu,Yanji Zhu,Lei Chen,Yue Sun,Meng Zhang,Huaiyuan Wang
Heteroatom modified catalyst applying for the two-electron oxygen reduction reaction has the potential application for efficient on-site production of H 2 O 2 . At present, state of the art catalyst synthesis is often energy-intensive and tends to destroy the original structure of heteroatoms. Based on the above considerations, Co-O, pyrrolic N structures co-modified graphite felt catalyst (Co-PDA-GF) is successfully synthesized by a simple two-step electrochemical method . Interestingly, the introduction of Co 2+ during the dopamine (DA) polymerization process changes the surface morphology of GF from a “thin-film” like to an “ant-nest” like. The cumulative H 2 O 2 concentration achieves 421 mg L −1 in 6 h test time, which is 16 times higher than that of R-GF, and the Methylene blue (MB) in-situ removal rate reaches 97.2% within 3 h. The enhanced H 2 O 2 yield of Co-PDA-GF catalyst is attributed to the increased oxygen-containing functional groups (-COOH, -C-O-C) and defect structures , and most importantly, Co-O and pyrrolic N synergistic modulation effects on local electronic modulation. This work provides new insights on DA polymerization morphology control and designing of high-efficient 2e − ORR catalyst with a low-energy method.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Manlin Zhu,Wangfeng Cai,Hongbo Wang,Leqiu He,Yan Wang
A morphologically adjustable metal-organic framework (MOF) template and a unique hierarchical structure show improved electrochemical performance of electrode materials for supercapacitors . Herein, Zn/Co-MOF-derived zinc-cobalt oxide/nickel cobalt layered double hydroxides (Zn-Co-O/NiCo-LDH) hierarchical core/shell nanostructures on nickel foam (NF) were synthesized by simple methods and exhibited high specific capacitance. The results showed that both the reasonable morphology of the MOF-templated continuous nanosheet network and synergy between transition bimetallic oxides and transition bimetallic hydroxide played an important role in improving the electrochemical properties . Hence, the as-prepared Zn-Co-O/NiCo-LDH battery-type electrode exhibited excellent specific capacitance of 2275.2 F/g at 1 A/g and remarkable cycling stability of 82.4% capacitance retention after 5000 cycles. Moreover, the as-prepared Zn-Co-O/NiCo-LDH was used as the positive electrode to assemble a hybrid supercapacitor (HSC) device, which attained a distinguished energy density of 44.5 W h/kg at a power density of 800 W/kg and satisfactory stability (71.5% retention after 5000 cycles). It was concluded that MOF-templated core/shell heterostructures in electrode materials have broad prospects and great potential for energy storage.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Tianhao Yu,Peng Gao,Yu Wang,Maidina Muhetaer,Hong Du
In response to the limitations of slow reaction kinetics and elevated overpotentials in the OER, a novel core–shell structured electrocatalyst, termed NiCo–ZIF-67@Fe–Co–Ni-PBA or NiCo–ZIF@PBA, has been developed. This material demonstrates exceptional catalytic performance, exhibiting a minimal overpotential of approximately 188 mV at 10 mA cm–2, alongside a Tafel slope of 109 mV dec–1. Its robust stability in a 1 M KOH solution during the OER operations is noteworthy. Theoretical insights from DFT calculations reveal that a Co–O–Fe bridging configuration within NiCo–ZIF@PBA lowers the energy barrier for the reaction to 1.79 eV, a significant reduction from 2.67 eV observed with NiCo–ZIF-67. The improvement in electrochemical performance is primarily due to the emergence of Co3+ ions, which results from the efficient charge transfer occurring at the interface of the PBA and NiCo–ZIF core–shell structure. These findings suggest a promising strategy for designing advanced core–shell materials for electrocatalytic applications.
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