ACS Applied Materials & Interfaces
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2017
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IF 7.504
Yu-Zhen Li,Tong-Tong Li,Wei Chen,Yan-Yan Song
Compared to natural enzymes, nanomaterial-based artificial enzymes have attracted immense attention because of their high stability and cost-effectiveness. In this study, cobalt nitride (Co4N) as a noble-metal-free artificial enzyme exhibiting highly intrinsic peroxidase-like activity and good stability was reported. Kinetic studies revealed that the resultant Co4N nanowires (NWs) exhibited a stronger affinity for 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2 than HRP. Compared to Co3O4 NWs, Co4N NWs exhibited highly improved catalytic activities, with H2O2 exhibiting an apparent Km approximately 2 orders of magnitude less than that of Co3O4. In particular, the peroxidase-like activity of Co4N was maintained well over a wide range of temperatures and ionic strength. A Co4N-based method was further developed for the detection of glucose with good sensitivity and reliability. Because of advantages such as easy storage, cost-effectiveness, high sensitivity, and outstanding stability, Co4N NWs demonstrate the potential for replacing noble-metal-based peroxidase mimetics in a wide range of promising applications.
研究领域:
生物化学
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材料科学
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医学诊断
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产品关联
DOI
PubMed
高影响因子
DIAMOND AND RELATED MATERIALS
·
2024
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IF 4.3
Yu Wang,Yanling Wang,Yunmei Du,Yanru Liu,Volodymyr Turkevych,Lei Wang
Transition metal nitrides (TMNs) have attracted great attention as ideal active materials in the field of electrocatalysts in recent years due to their excellent electrical conductivity, wide band gap and adjustable morphology. Pure phase Co 4 N nanoparticles encapsulated nitrogen-doped carbon (NC) nanotubes (Co 4 N@NC) were in-situ synthesized by one-pot method. In this paper, the morphology of carbon nanotubes is controlled by adjusting the pyrolysis time, so that more active sites are exposed on carbon nanotubes. Thus, the cobalt nitride catalyst with excellent catalytic performance for hydrogen evolution reaction (HER) in acidic electrolyte was obtained. In summary, due to the protection of mesoporous nitrogen-doped carbon to Co 4 N nanoparticles, large electrochemically active surface area, good conductivity and more exposed active sites, Co 4 N@NC possesses excellent HER performance in acidic electrolytes. The overpotential of Co 4 N@NC at the current density of 10 mA cm −2 is 117 mV (η 10 ), and it shows long-term stability in 0.5 M H 2 SO 4 solution for 50 h. This study provides a strategy for the development of catalysts for the controllable synthesis of high-performance transition metal nitrides.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 9
·期 3
·1655-1662
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IF 11.301
Mengjie Lu,Duo Chen,Boran Wang,Ruiqing Li,Dong Cai,Haoran Tu,Hang Yang,Yupu Zhang,Wei Han
Developing high-efficiency non-precious electrocatalysts for alkaline hydrogen evolution reaction (HER) is critical for practical application in water splitting. Abundant HER electrocatalysts exhibit high activity in acids, but deliver inferior performance in alkalis due to sluggish kinetics. Herein, motivated by the promoter CeO2 (rich in oxygen vacancies) that can modulate the electronic structure of materials, a high-efficiency catalyst of Co4N nanowires by coupling CeO2 vertically grown on Ni foam (Co4N–CeO2/NF) is prepared by composition control and interface engineering. Anchoring CeO2 into Co4N will endow the catalyst with superhydrophilic and superaerophobic properties, and simultaneously promote water adsorption/dissociation, which dramatically boost the alkaline HER performance. The as-synthesized self-supported Co4N–CeO2/NF electrode exhibits fairly low overpotentials of 52 and 149 mV at current densities of 10 and 100 mA cm−2 for HER in 1.0 M KOH electrolyte, respectively. Furthermore, after a long-time operation of 24 h at a fixed high current density of 100 mA cm−2, the required overpotential is increased only by 4 mV, showing the extraordinary long-time durability and promising potential in mass applications. This work will provide an effective strategy for rational design and activity enhancement of other non-precious metal-based HER electrocatalysts.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 48
·24767-24772
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IF 9.931
Rui-Qing Li,Pengfei Hu,Meng Miao,Yongle Li,Xiang-Fen Jiang,Qiang Wu,Zhen Meng,Zheng Hu,Yoshio Bando,Xue-Bin Wang
Obtaining a high-performance nonprecious electrocatalyst for oxygen and hydrogen evolution reactions (OER and HER) under mild conditions is highly desirable yet challenging. Transition metal nitrides are emerging as cost-effective substitutes for state-of-the-art noble metal based catalysts, but large OER overpotentials plague these nitrides. Herein, we developed the heterostructure of CoO-domain-anchored Co4N nanowhiskers as an effective bifunctional electrocatalyst for both OER and HER in neutral media. The exterior CoO targets OER, and the CO4N matrix is active for HER. The periodically-aligned {111} crystalline planes between Co4N and CoO provide good electron transport through their interface. The heterostructure performs dual functions of elevating activity and diminishing interior resistance of the catalyst. Moreover, the porous metallic Co4N nanowhiskers were integrated on a nickel foam, and this configuration contributes an arterial channel for collecting current as well as a spacious surface area for increasing the reaction cross section for heterocatalysis. These advantages actuate our bifunctional 3D catalytic electrode to achieve low OER and HER overpotentials in neutral systems. It finally provides an unprecedentedly low cell voltage (1.79 V for 10 mA cm−2) for catalyzing overall water splitting in neutral media.
研究领域:
电化学
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材料科学
✓ 已验证
DOI
高影响因子
CARBON
·
2019
·
IF 7.466
Lulu Chen,Yelong Zhang,Xiangjian Liu,Ling Long,Siyu Wang,Xiaolong Xu,Minchao Liu,Wenxiu Yang,Jianbo Jia
The development of transition metal nitrides/carbon hybrids with well-organized morphology, outstanding efficiency and durability for Zn-air batteries are of great urgency. Herein, a morphology-controlled strategy to efficiently fabricate uniform Co 4 N nanoparticles anchored on N -doped carbon (Co 4 N@NC-m) is reported. The diameters and distribution of Co 4 N nanocrystals can be tuned to be homogeneous profited by abundant N sources in melamine. Moreover, thanks to the advantages of higher nitrogen doping content, better electrical conductivity , higher degree of graphitization , and larger electrochemical surface area, Co 4 N@NC-m possesses excellent oxygen reduction reaction (half-wave potential of 0.87 V) and oxygen evolution reaction (overpotential of 398 mV at 10 mA cm −2 ) activities in basic solution. The Zn-air battery fabricated with Co 4 N@NC-m owns higher open circuit voltage (1.490 V), larger power density, and better rechargeability than those of the commercial IrO 2 + 20% Pt/C catalysts, which proves the potential application in practical energy conversion devices.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Liyan Wang,Zhaokun Wang,Liang Chu,Mu Yang,Ge Wang
The design of transition metal nitrides with excellent oxygen evolution reaction and 5-hydroxymethylfurfural oxidation reaction (HMFOR) is of great significance to achieve the goal of "carbon peaking and carbon neutrality". Herein, Fe-doped bimetallic nitride Fe x Co 1-x ) 4 N was prepared by a simple electron regulation strategy. The introduction of Fe changes the electronic structure of Co and optimizes the adsorption energies of *OH, reduces the potential barrier for the generation of *OOH as a potential-determining step and thus increases the intrinsic OER activity of Co 4 N. In addition, Fe substitution of some of the Co atoms gives (Fe x Co 1-x ) 4 N a higher electrochemical active surface area, which accelerates the electron transfer efficiency and improves the electrical conductivity. The overpotential for (Fe x Co 1-x ) 4 N-0.9 to reach a current density of 10 mA cm −2 in 1 M KOH is only 271 mV. When in 1 M KOH + 50 mM HMF condition, (Fe x Co 1-x ) 4 N-0.9 requires only 1.37 V to reach a current density of 10 mA cm −2 . This work provides practical guidance for developing bifunctional transition metal electrocatalysts with excellent OER and HMFOR activity.
研究领域:
材料科学
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电催化
·
能源转换与存储
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Lichao Li,Tongrui Shao,Yang Su,Xiaodong Wang,Jian Lin
Water gas shift (WGS) reaction is crucial for removing CO impurity in industrial hydrogen production. Noble-metal-free Co-based species mainly serve as a support rather than dominant sites for this reaction. Here, a bulk Co 4 N nanospheres (Co 4 N-NS) catalyst is prepared via temperature programmed nitriding using Co 3 O 4 nanosphere precursor for low-temperature WGS reaction. It is found that the CO conversion can achieve 97.6% at 240°C, and the thermodynamic equilibrium conversion is reached at 250°C, which is unprecedentedly reported for Co-based catalysts. Moreover, the reaction rate reaches 19.84 mmol CO g cat −1 h −1 with a better stability, 4.5 times higher than that on Co 4 N-C from commercial Co 3 O 4 precursor. The characterizations and kinetic studies show that Co 4 N-NS enhances the H 2 O activation and promotes the CO adsorption, which renders a lower activation energy compared to Co 4 N-C for the WGS reaction. This study offers insights for designing cost-effective WGS catalysts with transition metal nitrides.
研究领域:
催化化学
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材料科学
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化学工程
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Physics
·
2020
·
IF 10.443
Xiao Hui Chen,Qing Zhang,Li Li Wu,Li Shen,Hong Chuan Fu,Juan Luo,Xiao Lin Li,Jing Lei Lei,Hong Qun Luo,Nian Bing Li
Heretofore, the metal elements constituting the electrolyzed water catalysts are almost all Fe, Co, and Ni, and the accelerator elements are V, W, Ce, etc., but there is a lack of exploration for other elements. Niobium (Nb) is a promising promoter due to its complex chemical properties and the ability to react with many elements to form abundant compounds. Taking Co 4 N as the research case, this work incorporates Nb atoms to tune the d orbital of metallic Co 4 N nanowires . Experimental results and density functional theory calculations show that due to the adjustment of Nb atoms, the d-band center of Co 4 N moves down, which helps facilitate the desorption of H 2 . At the same time, abundant Co 3+ active sites are generated on the surface of Nb–Co 4 N, which is crucial for the formation of oxygen evolution reaction (OER) intermediates (∗OOH). Nb-regulated Co 4 N nanosheets on the three-dimensional Ni foam (Nb–Co 4 N/NF) drives the current density of 20 mA cm −2 at a low overpotential of 90 mV for hydrogen evolution reaction and 273 mV for OER, respectively. This work inspires a novel idea for the rational design and synthesis of highly efficient electrocatalysts composed of novel less used elements for overall water splitting.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Peiyun Zhou,Guangtong Hai,Gongchi Zhao,Rushuo Li,Xiubing Huang,Yunfeng Lu,Ge Wang
Developing multifunctional electrocatalysts with excellent hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and 5-hydroxymethylfurfural oxidation reaction (HMFOR) activities will contribute to "carbon neutrality". Here, CeO 2 is introduced into the Co 4 N system as an "electron pump" to attract electrons to transfer from Co 4 N to CeO 2 . The interface electronic structure optimization enables Co 4 N@CeO 2 to exhibit excellent HER, OER, and HMFOR performance. Specifically, to deliver 10 mA cm −2 current density, (1) it only requires low overpotentials of 49 and 263 mV for HER and OER in 1.0 M KOH, respectively; (2) it merely needs an ultra-low potential of 1.22 V RHE for HMFOR in 1.0 M KOH + 300 mM HMF, which is 273 mV lower than the required potential in 1.0 M KOH. Theoretical calculation results show that the introduction of CeO 2 effectively reduces the barriers for potential-determining steps of HER and OER, and optimizes OH - adsorption to promote the HMFOR process.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Fengmei Wang,Huimin Zhao,Yiru Ma,Yu Yang,Bin Li,Yuanyuan Cui,Ziyang Guo,Lei Wang
Designing the highly catalytic activity and durable bifunctional catalysts toward oxygen reduction/evolution reaction (ORR/OER) is paramount for metal–air batteries . Metal–organic frameworks (MOFs)-based materials have attracted a great deal of attention as the potential candidate for effectively catalyzing ORR/OER due to their adjustable composition and porous structure . Herein, we first introduce the Mn species into zeolitic-imidazole frameworks (ZIFs) and then further pyrolyze the Mn-containing bimetallic ZIFs to synthesize core-shell-structured Co@Co 4 N nanoparticles embedded into MnO-modified porous N-doped carbon nanocubes (Co@Co 4 N/MnO NC). Co@Co 4 N/MnO NC exhibits the outstanding catalytic activity toward ORR and OER which is attributed to its abundant pyridinic/graphitic N and Co 4 N, the optimized content of MnO species, highly dispersed catalytic sites and porous carbon matrix. As a result, the Co@Co 4 N/MnO NC-based Zn–air battery exhibits enhanced performances, including the high discharge capacity (762 mAh g Zn −1 ), large power density (200.5 mW cm −2 ), stable potential profile over 72 h, low overpotential (<1.0 V) and superior cycling life (2800 cycles). Moreover, the belt-shaped Co@Co 4 N/MnO NC cathode-based Zn–air batteries are also designed which exhibit the superb electrochemical properties at different bending/twisting conditions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Bo Cao,Baocang Liu,Zichao Xi,Yan Cheng,Xuan Xu,Peng Jing,Rui Cheng,Shien-Ping Feng,Jun Zhang
Transition metal nitrides (TMNs) have received special concern as important energy storage materials, owing to their high conductibility, good mechanical strength, and superior corrosion resistance. However, their insufficient capacitance and poor cycling stability limit their practical applications for supercapacitors. Here, a novel three-dimensional (3D) self-supported integrated electrode consisted of porous nanowall arrays of ultrafine cobalt nitride (Co4N) nanoparticles encapsulated in a lanthanum oxycyanamide (LOC) matrix on carbon cloth (Co4N@LOC/CC) for outstanding electrochemical energy storage is rationally designed and fabricated. The 3D monolithic configuration of porous nanowall arrays facilitates the mass/charge transfer, the exposure of electroactive sites, and the enhancement of electrical conductivity. Meanwhile, the unique core–shell structure of Co4N@LOC can prevent ultrafine Co4N nanoparticles from sintering, agglomeration, and oxidation and promotes electron transfer dynamics during the redox reaction, meanwhile enhancing the stability of the electrode. Additionally, the synergy of Co4N and LOC can result in an efficient electron/ion transport in the process of the charge–discharge. Because of these features, the Co4N@LOC/CC electrode displays superior specific capacitance (895.6 mF cm–2 or 613.4 F g–1 at 1 mA cm–2) and admirable cycling durability (87.9% capacitance reservation after 10 000 cycles), surpassing the majority of nitride-based electrodes reported thus far. Furthermore, after being assembled into an asymmetric supercapacitor using active carbon (AC) as an anode, the obtained Co4N@LOC/CC//AC/CC device displays a high energy density of 41.7 Wh kg–1 at the power density of 875.8 W kg–1 with a high capacitance reservation of 87.6% after 5000 cycles at 2 mA cm–2. This work offers an efficient approach of combining TMNs with rare earth compounds to enhance the capacitance and stability of TMNs for supercapacitor electrodes.
研究领域:
材料科学
·
能源存储
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Yaxin Zheng,Zexiu An,Weihua Liu,Minghua Wang,Yichun Ren,Dongchen Yang,Wei Gao,Ningzhao Shang,Jinlin Zhang,Chun Wang,Shutao Gao
Nitrogen vacancy incorporation into Co 4 N-600 upshifts the D-band center and facilitates the generation of Co IV =O. • The Co 4 N-600/PMS system yields a modified kinetic rate constant of 300.6 min⁻ 1 M⁻ 1 . • Rapid degradation of different types of pollutants within Co 4 N-600/PMS system. High‑valent cobalt-oxo species (Co IV =O) have been demonstrated to exhibit efficient degradation capability toward emerging contaminants (ECs). However, the 3d 7 electronic configuration of Co(II) sites in Co‑based catalysts severely restricts their binding affinity to the terminal oxygen of peroxymonosulfate (PMS), which is unfavorable for the generation of Co IV =O. Herein, we report a nitrogen vacancy (Nv)‑rich cobalt nitride nanozyme Co 4 N-600. The introduction of Nv markedly reduces the d‑electron occupancy of Co, upshifts the d‑band center, and promotes the formation efficiency of Co IV =O. Remarkably, employing 150 mg L −1 peroxymonosulfate (PMS) as the oxidant, the Co 4 N-600 nanozyme achieves complete degradation of 10 mg L −1 imidacloprid within 10 min at an ultralow catalyst loading of 1 mg L −1 , yielding an excellent modified kinetic rate constant of 300.6 min −1 M −1 . These findings establish d -band center engineering as an effective strategy for boosting the catalytic performance of nanozymes by promoting the generation of high-valent metal-oxo (HVMO) species. Download: Download high-res image (179KB) Download: Download full-size image
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DOI
PubMed
高影响因子
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