ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 5
·1857-1865
·
IF 4.478
Sun Liping,Yan Yong,Chen Shuai,Zhou Zijue,Tao Wei,Li Chao,Feng Yi,Wang Feng
Biothiol detection is of great importance for clinical disease diagnosis. Previous nanozyme-based colorimetric sensors for biothiol detection showed unsatisfactory catalytic activity, which led to a high detection limit. Therefore, developing new nanozymes with the high catalytic activity for biothiol detection is extremely necessary. Recently, single-atom nanozymes (SAzymes) have attracted much attention in biosensing due to their 100% atom utilization and excellent catalytic activity. Most previous works focus on the peroxidase-like activity of Fe-based SAzymes by using unstable and destructive H 2 O 2 as the oxidant. It is essential to develop new SAzymes with high oxidase-like activity for biosensing to break through the limitation. Herein, Co–N–C SAzymes with high oxidase-like activity are explored. Furthermore, Co–N–C SAzymes are used as a biosensor for colorimetric detection of biothiols (GSH/Cys) based on the inhibition of thiols toward the oxidase-like activity of Co–N–C SAzymes, which showed high sensitivity with a low detection limit of 0.07 µM for GSH and 0.06 µM for Cys. Besides, the method showed good reproducibility and high selectivity against other amino acids. This work offers new insights using Co–N–C SAzymes in the biosensing field.
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ENERGY & FUELS
·
2023
·
IF 5.3
Dongju Fu,Ziyue Zhu,Shaojun Gao,Hui Qi,Xuguang Liu,Weifeng Liu,Shaozhong Zeng
In this paper, hollow Co/N-C@NiCo2O4 spheres assembled by nanoparticles were developed as efficient bifunctional catalysts for zinc–air batteries. The hollow structure is synthesized with ZIF-67 as a reactant template. NiCo-LDH grown on the ZIF-67 surface maintains its structural integrity during heat treatment and reduces the agglomeration of the material, which promotes charge transport during the catalytic process. The hollow structure has a specific surface area of 124.3 m2 g–1 with rich catalytic active sites. As expected, the power density of the Co/N-C@NiCo2O4-based Zn–air battery is 176 mW cm–2 and the specific capacity is 745 mAh g–1, with 1.45 V open-circuit voltage and 100 h cycling life, much better than those of the 20% Pt/C-RuO2-based Zn–air battery (1.42 V, 133 mW cm–2, 721 mAh g–1).
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ChemElectroChem
·
2022
·Vol. 9
·期 11
·e202200375
·
IF 4.782
Junting Sun,Jiaxiang Jin,Yatao Chang,Jing Wang,Qindong Zhang,Junjie Guo
Graphical Ramping rate matters in pyrolysis : Hybrid Co/N−C electrocatalysts were synthesized using NaCl as template via direct pyrolysis method. Ramping rates during pyrolysis was evidenced to affect the porosity and composition of the obtained electrocatalysts due to the different diffusion rates and decomposition reaction of precursors, which have significant influences on their catalytic activities toward oxygen reduction. Pyrolysis is a necessary procedure for synthesizing carbon-based nonprecious metal electrocatalysts via stimulating interaction and carbonization of precursors. In this work, ramping rates that correlated with thermal gradient has been investigated to reveal the configuration evolution of the precursors. Spectra characterizations demonstrated that ramping rates affected decomposition and aromatization of precursors. Increasing ramping rates improved the percentage of doped nitrogen and defects, promoting dispersion of Co atoms in the carbonaceous matrix and increasing density of active sties. In addition, the size variation of NaCl template under different ramping rates modifies the porous structure of Co/N−C electrocatalysts, greatly increasing the percentage of macropores and micropores at rapid ramping rates. As a result, electrocatalysts obtained at 5 °C min −1 exhibit comparable catalytic activity to that of Pt/C due to highly dispersed active sites and rational percentage of porosity, facilitating the sufficient reaction of oxygen along the catalysts. These results shed lights on regulating physical properties of carbonaceous electrocatalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Rongcheng Mo,Xiaoran Zhang,Zhenyu Chen,Shangli Huang,Yanjie Li,Lizhe Liang,Zhi Qun Tian,Pei Kang Shen
Developing platinum-based nanoparticles on carbon catalysts with high activity and stability for oxygen reduction reaction (ORR) is of great significance for the practical application of fuel cells. Herein, a synchronous strategy of preparing nano-sized PtCo supported on atomic Co and N co-doped carbon nanorods (PtCo/Co–N–C NR) was developed to replace the conventional method of impregnating Pt sources into ready-made carbon materials , in which metal-organic frameworks (MOFs) with Co and Zn ions of rhombic dodecahedron were first prepared using 2-methylimidazole as building block and then their morphology was transformed into porous nanorods via the reduction of Co ions to Co–B–O complex in the MOFs by NaBH 4 ; subsequently, Pt was deposited on the Co–Zn MOF nanorods through the displacement reaction of PtCl 6 2 - and metallic Co and coordination between MOF and PtCl 6 2 - ; after pyrolysis and acid-leaching process, highly dispersed PtCo/Co–N–C NR was obtained. Attributed to its unique characteristics of hierarchical pore structure , uniform PtCo alloy nanoparticles with the average size of 7.0 nm and strong supporting interaction effect, the catalyst exhibits high ORR activity and stability with the mass activity of 577.0 mA mg −1 Pt and specific activity of 1.4 mA cm −2 at 0.9 V vs RHE in 0.1 M HClO 4 , which is about 3.6 times and 3.5 times high than that of commercial Pt/C catalyst respectively. This strategy would provide a flexible route to develop highly active and stable ORR electrocatalysts with various morphologies for optimizing the exposure of active sites.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yijie Feng,Wenjiao Sang,Zhiyi Deng,Shiyang Zhang,Cuihua Li
Co-N-C@SiO 2 with Co, N doped carbon as core and SiO 2 as shell was successfully synthesized by template method, and SiO 2 shell was about 43 wt%. Impressively, the SiO 2 shell increased the active sites of the core in Co-N-C@SiO 2 preparation, and reduced the loss of active sites during use. Co-N-C@SiO 2 /PMS was a 1 O 2 dominated non-radical reaction, which was less interfered by solution pH and water constituents. In addition, Co-N-C@SiO 2 possessed better cycling performance compared with Co-N-C. Finally, the possible SMX degradation pathways were presented based on the identified intermediate products.
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CATALYSIS TODAY
·
2019
·
IF 4.888
Mantang Chen,Nan Wang,Lihua Zhu
Single-atom catalysts with a maximum atomic utilization are promising in wastewater treatment. Herein, a single-atom dispersed Co-N-C catalyst was prepared by a calcination-acid treatment method. The obtained Co-N-C was confirmed to possess excellent performances of both adsorption and catalytic ability of activating peroxymonosulfate (PMS). It was found that the adsorption performance was related to the surface area and pore volume and the removal of bisphenol A (BPA) was determined by the defect density of the catalyst. It was observed that a calcination temperature of 900 °C yielded the best Co-N-C catalyst named Co-N-C-900. All the added BPA (80 mg L −1 ) was completely degraded in 3 min by using 0.5 g L −1 Co-N-C-900 and 0.3 g L −1 PMS with a degradation rate constant ( k ) of as high as 2.81 min −1 . In this single-atom catalytic system, the main reactive species were confirmed to be singlet oxygen. A mechanism study suggested that the fast and efficient degradation of BPA was attributed to the synergistic effect between fast adsorption of mesoporous carbon and efficient catalysis of single-atom Co-N x complex.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Qingqing Li,Zhiwei Sun,Yilin Wei,Zixu Ma,Liucheng Wang,Renfeng Nie
Reversible hydrogen storage via Liquid organic hydrogen carriers (LOHCs) is one of the key technologies for efficient utilization of hydrogen energy. How to construct efficient dehydrogenation/hydrogenation catalysts that enable low-temperature catalysis still remains challenging. Herein, we present the design and construction of single-atom Co-N-C(x) catalysts allowing significantly improved acceptorless dehydrogenation of 1,2,3,4-tetrahydroquinoline (THQ). By varying the ligand/Co ratio, the optimal Co-N-C(1.5) can achieve 97.5% dehydrogenated product and 0.82 h −1 TOF value at ambient temperature, overperforming many reported non-noble metal even noble metal catalysts. This catalyst exhibits good recyclability and substrate versatility, enabling ambient temperature dehydrogenation of various N-heterocycles and efficient reverse hydrogenation of aromatic N-heterocycles, thus achieving the loop of reversible hydrogen storage. The active catalyst centers consist of specific Co-N x moieties and nitrogen species within the carbon support. Controlled experiments reveal that the different performance of Co-N-C(x) is determined by density of the Co-N x , and the rate-determining step of THQ dehydrogenation is correlated with the bond cleavages in surface-bound THQ. This work offers a promising pathway for energy-efficient and cost-effective hydrogen energy utilization under practical conditions.
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Energy & Environmental Materials
·
2021
·Vol. 5
·期 2
·543-554
·
IF 15.122
Yu Ma,Ding Chen,Weijun Li,Yapeng Zheng,Lin Wang,Gang Shao,Qiao Liu,Weiyou Yang
The design of efficient cathode with great cycle performance, high flexibility, and low cost is essential for the commercialization of zinc–air battery (ZAB). Herein, we report the exploration of freestanding bifunctional cathode with rationally designed structures, namely, tiny Co nanoparticles embedded in N-doped carbon nanofiber aerogels, which have desired features including uniform Co dispersity, balanced distribution of N-C species, hierarchically porous structure with increased fraction of meso- to micropores, and moderate amounts of defects. Accordingly, the as-fabricated cathodes exhibit positive half-wave potential of 0.82 V for oxygen reduction and small overpotential of 350 mV at 10 mA cm −2 for oxygen evolution, respectively, which deliver smaller reversible oxygen electrode index (0.76 V) than the commercial Pt/C+RuO 2 (0.80 V) and most Co-based electrocatalysts ever reported. Impressively, the as-constructed liquid rechargeable ZAB behaves high peak power density (160 mW cm −2 ), large specific capacity (759.7 mAh g −1 at 10 mA cm −2 , tested after 120 h of OCV tests), and robust stability over 277 h. Moreover, the as-assembled quasi-solid-state ZAB using such freestanding cathode represents excellent mechanical flexibility and outstanding cycle performance, regardless of being serviced under extremely bending conditions from 0° to 180°, underscoring their promising applications as durable bifunctional cathode for portable metal–air batteries.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 10
·104502
·
IF 3.721
Guofeng Liang,Jilin Huang,Jiawang Li,Yinlong Wu,Guoju Huang,Yan Qi Jin,Hongbin Zeng,Hao Zhang,Jian Chen,Yanshuo Jin,Nan Wang,Fangyan Xie,Hui Meng
Transition metal and nitrogen co-doped carbon-based nanomaterial has been used as non-precious metal catalyst for oxygen reduction reaction (ORR). In this work, bamboo-like carbon nanotubes structured FeCo/N/C electrocatalyst is proved to show much enhanced performance compared with Co/N/C. MIL-53 (Fe) is used as iron source, MIL-53 (Co) is used as cobalt source and ZIF-8 as carbon source. The ball-milling procedure plays a significant role for the distribution of Fe and Co component and the formation of carbon nanotubes, which is believed to enhance the catalytic performance due to abundant electrocatalytic active sites and efficient mass transfer. The as prepared sample obtained by optimized preparation conditions exhibits outstanding ORR activity in acid solution with an onset potential of 0.96 V vs RHE (reversible hydrogen electrode), half-wave potential of 0.78 V, and a current density of 0.575 m A cm−2 at 0.7 V in a H2-O2 fuel cell test, which provides an ideal viewpoint to develop highly efficient catalyst for the oxygen reduction reaction. The high ORR performance could be attributed to the synergistic effect between Fe and Co and the high conductivity and mass transfer of the carbon nanotube.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Yue Han,Xuehui Tang,Xiangyu Wu,Hongyi Shi,Lei Huang,Lei Wei,Mingmin Li,Yue Zhang
l -Cysteine ( l -Cys) is a significant biomarker for various diseases, including liver disease, skin disorders, and Parkinson’s disease, making its detection crucial for diagnostic purposes. In this study, we present a novel colorimetric sensing platform for l -Cys detection. Using ZIF-8 as a precursor, a cobalt-based single-atom catalyst (Co-N-C) was synthesized through pyrolysis, adsorption, and activation processes. The resulting Co-N-C catalyst exhibited remarkable oxidase-like (OXD-like) activity, effectively facilitating the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to form oxTMB, which resulted in a distinct blue color. However, due to its strong reducibility, l -Cys can scavenge reactive oxygen species (ROS) generated by the Co-N-C catalyst, thus inhibiting the oxidation of TMB. By monitoring the color change in the solution, we developed a highly sensitive colorimetric assay for l -Cys detection. The assay demonstrates excellent selectivity and has a detection limit of 0.1 µM, with a linear detection range from 0.1 to 10 µM. This work offers an efficient approach for detecting l -Cys and establishes a new framework for designing high-performance nanozymes.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Deqiang Kong,Yueshuai Wang,Yong Yan,Zongge Li,Yue Lu,Ge Chen
Advancing the two-electron (2e - ) oxygen reduction reaction (ORR) in acidic media is pivotal for sustainable, on-demand hydrogen peroxide (H 2 O 2 ) production, but remains challenged by insufficient activity/selectivity at industrially relevant high current densities. We present a breakthrough catalyst design featuring cobalt atomic sites embedded in curved nitrogen-doped carbon layers (c-Co-N-C). This architecture achieves nearly 90 % H 2 O 2 selectivity across a wide potential window, delivering 11.70 mol g⁻¹ h⁻¹ productivity at 300 mA cm −2 with 80 % Faraday efficiency in flow cell tests. Particularly, the catalyst maintains a stable 300 mA cm −2 operation under 1.9 V cell voltage (surpassing prior-art systems by 0.2 V) for 120 h in a PEM electrolyzer, producing pure-phase H 2 O 2 (4.1 wt%). Through integrated experimental and computational analysis, we reveal two complementary enhancement mechanisms: first, the finite element simulations quantify the enhanced interfacial electric field that concentrates protons and dissolved oxygen; then, the density functional theory (DFT) calculations indicate a downshift in Co d -band center optimizes *OOH adsorption while suppressing O-O bond cleavage. This work establishes curvature engineering as a universal design strategy for advanced catalysts through controlled structural modification, opening new pathways for sustainable chemical synthesis.
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MICROCHIMICA ACTA
·
2026
·Vol. 193
·期 5
·294
·
IF 5.4
Xu Xiaowen,Liu Tiandi,Ma Tenghe,Li Tengfei,Wang Jing
A smartphone-assisted colorimetric sensing platform was developed for the sensitive detection of sulfites based on a cobalt single-atom nanozyme (Co-N-C). The nanozyme was synthesized via high-temperature pyrolysis of bimetallic Zn/Co-ZIF precursors, resulting in atomically dispersed Co active sites anchored on a nitrogen-doped carbon framework. Benefiting from the well-defined catalytic centers, Co-N-C exhibits exceptional oxidase-like activity, efficiently catalyzing the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) into a blue product (oxTMB). The presence of sulfites triggers rapid discoloration through a dual mechanism involving reactive oxygen species (ROS) scavenging and the direct reduction of oxTMB. Under optimized conditions, the proposed assay demonstrates a wide linear range of 0.5–80 µM with a low detection limit of 0.066 µM. To eliminate potential interference from biothiols such as glutathione, a selective masking strategy using N-(2-hydroxyethyl)maleimide (HEMI) was introduced. Furthermore, integration with smartphone-based RGB analysis enables portable and instrument-free quantification. The platform was successfully applied to real food samples (white sugar, liquor, and bean vermicelli), yielding satisfactory recoveries of 92.6%-104.0%. This work highlights the potential of single-atom nanozymes in developing low-cost, portable sensing platforms for practical food safety monitoring.
Section
Graphical abstract
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危险品化学品经营许可证（带存储）