Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 48
·25378-25384
·
IF 8.867
Tanyuan Wang,Chao Wang,Yue Jin,Anna Sviripa,Jiashun Liang,Jiantao Han,Yunhui Huang,Qing Li,Gang Wu
Transition metal phosphides are often studied as hydrogen evolution reaction cathode catalysts, but scarcely as oxygen evolution reaction (OER) anode catalysts for water oxidation. Herein, we report a new amorphous Co0.63Fe0.21P0.16 OER catalyst, which was prepared through a one-step solvothermal process. This catalyst exhibits extraordinary OER catalytic activity in alkaline media and is superior to the state of the art IrO2 in 1.0 M KOH, capable of yielding a current density of 10 mA cm−2 at an overpotential of only 217 mV. This newly achieved high activity outperforms most reported transition metal phosphide catalysts. During the OER, the surface layers of the Co0.63Fe0.21P0.16 nanospheres (200–500 nm) are oxidized, which show the typical Tafel slope of oxides around 40 mV dec−1. The in situ formation of surface Co oxides in the catalysts during the OER along with an optimal doping of Fe are found to be crucial for their remarkable activity. In particular, the metal-rich amorphous phosphide cores, i.e., substrates, probably contribute to OER performance of the catalysts due to their high electrical conductivity. This new type of surface oxidized amorphous transition metal phosphide would provide a new pathway for the design of high-performance OER electrocatalysts.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Haixiang Shi,Yiyuan Xu,Tongming Su,Xuan Luo,Xinling Xie,Zuzeng Qin,Hongbing Ji
The surface acidity and structure of catalysts play crucial roles in cinnamaldehyde (CAL) selective hydrogenation to manufacture cinnamyl alcohol (COL). Herein, a Co–Fe-supported acidified bentonite catalyst (Co–Fe/ACBT) was prepared via sulfuric acid treatment of bentonite (BT) and the traditional impregnation method. The combination study, including FT-IR spectra of adsorbed pyridine and ammonia temperature-programmed desorption (NH3-TPD), showed that Co–Fe/ACBT has vast acidic sites mainly originating from surface unsaturated metal sites of ACBT, which prefer to adsorb polar >CO but not nonpolar >CC<. X-ray photoelectron spectroscopy (XPS) verified that the effect of electron transfer was significantly enhanced when the active metal was loaded on ACBT, leading to an increase in the electron cloud density of the Co species, which promoted the activation of >CO. Due to the modified electronic properties of Co species and abundant acidic sites, Co–Fe/ACBT exhibited a 90.5% conversion and 86.8% hydrogenation selectivity from CAL to COL, which are notably greater than those of the Co–Fe-supported bentonite catalyst (32.0% CAL conversion and 66.4% COL selectivity).
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2021
·
IF 4.098
Xiao-Lan Zhao,Jia-Li Liu,Fa-Ting Xie,Tong Yang,Rong Hu,Yun-Hui Yang
In this paper, a simple, rapid, and low-cost colorimetric method was designed based on Co/Fe-MOFs-iodide composite for the quantitative detection of H 2 S. It is know that iodide can improve the catalytic activity of bimetallic porous material Co/Fe-MOFs via adsorption into the framework of MOFs. Herein, we demonstrate a novel strategy to enhance the peroxidase-like activity of MOFs. Compared to horseradish peroxidase (HRP), the kinetic measurement results show that Co/Fe-MOFs-iodide exhibits excellent affinity to substrates, promoting electron transfer. Due to the synergetic effect of Co/Fe-MOFs and iodide, and rapid electron transfer process, Co/Fe-MOFs-iodide demonstrates improved peroxidase-like activity. As a proof-of-concept application, a novel, highly sensitive H 2 S colorimetric method is established with a detection limit (LOD) of 0.33 nM. In the absence of iodide, LOD is approx. 200-fold higher than that of the amplified colorimetric assay. The proposed method can also accurately detect traces of H 2 S in serum samples.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2026
·
IF 5.9
Huan Song,Le Song,Fangzhou Wu,Yonglei Xing,Xiaoyong Jin,Gang Ni,Xin Wang
Utilizing bimetallic synergy presents a promising approach for creating exceptionally effective catalysts for peroxymonosulfate (PMS) activation. In this study, a Co Fe bimetallic catalyst (Co8Fe1-P1-NC) was constructed by regulating the Co/Fe doping ratio and further introducing phosphorus doping. During PMS activation for phenol (Ph) degradation, Co8Fe1-P1-NC exhibited outstanding catalytic performance. Under the optimized conditions, the Co8Fe1-P1-NC/PMS system achieved complete removal of Ph within 2.5 min, with an apparent rate constant as high as 2.058 min −1 and a total organic carbon (TOC) removal efficiency of up to 80%. Combined results from quenching experiments, electron paramagnetic resonance (EPR), in situ Raman spectroscopy, electrochemical measurements, and premixing tests demonstrated that O 2 •− , 1 O 2 , high-valent metal species, and electron-transfer pathways collectively contributed to Ph degradation. Theoretical calculations indicate that Fe and P doping make the PMS adsorption energy more negative and elongate the O O bond (l O–O ), thereby facilitating PMS activation on the catalyst. Co8Fe1-P1-NC also showed excellent broad-spectrum degradation capability toward various phenolic pollutants, achieving complete removal within 3 min. These findings indicate that the combined regulation of metal active sites and electronic structure through bimetallic synergy and nonmetal doping can significantly enhance PMS activation efficiency, providing a new avenue for the design of high-performance catalysts.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Fang Liu,Weiyang Jin,Ying Li,Lekai Zheng,Yongchuan Hu,Xuewen Xu,Yanming Xue,Chengchun Tang,Hui Liu,Jun Zhang
The development of efficient non-precious metal catalysts to accelerate the oxygen evolution reaction (OER) kinetics is important for the development of water-derived hydrogen fuel. Iron-cobalt oxide ((Co, Fe) 3 O 4 ) is one of the most promising transition metal-based OER electrocatalysts under alkaline conditions, but its activity is unsatisfactory due to its limited active sites and poor electronic conductivity. Herein, self-supported (Co, Fe) 3 O 4 hierarchical nanosheet arrays with massive oxygen vacancies (denoted as V O -(Co, Fe) 3 O 4 /CC) are synthesized by a simple reduction method at room temperature. Oxygen vacancies can regulate the ratio of Co 2+ /Co 3+ , which leads to the modification of its electronic properties, and it also significantly improves the charge transfer ability and accelerates the reaction. Meanwhile, the unique hierarchical nanosheet arrays structure and abundant oxygen vacancies effectively adjust the number of OER active sites, which has a key role in developing a cost-effective oxygen electrode. Accordingly, V O -(Co, Fe) 3 O 4 /CC exhibits a relatively low overpotential of 286 mV at 10 mA cm −2 and a low Tafel slope of 41 mV dec −1 .
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JOURNAL OF APPLIED ELECTROCHEMISTRY
·
2016
·Vol. 47
·期 3
·361-367
·
IF 2.223
Xiao Mingshu,Zhang Zhonghui,Tian Yanping,Miao Yuqing,Wang Jiahai
Abstract In this work, the synthesis of Co–Fe–Se ultrathin nanosheet-fabricated microspheres was reported for the first time as electrocatalysts toward hydrogen evolution reaction (HER). The Co–Fe–Se ternary compounds exhibited high electrocatalytic activity of HER with low onset potential in acid media due to the high specific surface area of Co–Fe–Se ultrathin nanosheet-fabricated microspheres. The presence of multiwall carbon nanotubes improved the immobilization effect of Co–Fe–Se catalysts and electron transfer between catalysts and electrode surface, leading to the improved stability and HER electrocatalysis. The non-noble metal-based ternary compounds of Co–Fe–Se obtained from earth-abundant elements may enlighten a new way of exploring cost-effective catalysts for HER to develop hydrogen energy. Graphical Abstract
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 22
·15547-15554
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IF 3.3
Changyin Zhong,Yifei Yang,Yun Fang,Jun Chen,Bomin Feng,Hongbing Wang,Wenhua Luo,Yunxi Yao
Lanthanum oxide (La2O3) possesses superior reactivity during catalytic hydrogenation, but the intrinsic activity of La2O3 toward H2 adsorption and activation remains unclear. In the present work, we fundamentally investigated hydrogen interaction with Ni-modified La2O3. Hydrogen temperature programmed desorption (H2-TPD) on Ni/La2O3 shows enhanced hydrogen adsorption with a new hydrogen desorption peak at a higher temperature position compared to that on the metallic Ni surfaces. By systematically exploring the desorption experiments, the enhanced H2 adsorption on Ni/La2O3 is due to the oxygen vacancies formed at the metal–oxide interfaces. Hydrogen atoms transfer from Ni surfaces to the oxygen vacancies to form lanthanum oxyhydride species (H–La–O) at the metal–oxide interfaces. The adsorbed hydrogen at the metal–oxide interfaces of Ni/La2O3 results in improved catalytic reactivity in CO2 methanation. Furthermore, the enhanced hydrogen adsorption on the interfacial oxygen vacancies is ubiquitous for La2O3-supported Fe, Co, and Ni nanoparticles. Benefiting from the modification effect of the supported transition metal nanoparticles, the surface oxyhydride species can be formed on La2O3 surfaces, which resembles the recently reported oxyhydride observed on the reducible CeO2 surfaces with abundant surface oxygen vacancies. These findings strengthen our understanding of the surface chemistry of La2O3 and shed new light on the design of highly efficient La2O3-based catalysts with metal–oxide interfaces.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124383
·
IF 7.5
Zhengyan Liu,Xiaoli Su,Jie Li,Nan Jiang,Muhammad Imran,Yunxia Chen
A plasma-catalytic system coupled with floating electrode discharge with metal foam-supported catalysts was developed for efficient toluene degradation. The influences of different transition metal oxides (Co, Mn, Ce) loaded onto Fe foam (FF) substrates on the crystal structure, surface morphology and catalytic performance were systematically investigated. Catalysts were symmetrically placed on both sides of the floating electrode. Among the investigated metal oxides, Co was found to form a uniformly distributed CoFe 2 O 4 surface layer on the FF substrate, while Mn and Ce were heterogeneously dispersed as MnO 2 and CeO 2 , respectively. All metal-loaded catalysts enhanced the discharge power of the reactor, attributed to surface charge accumulation on metal oxides. The Co/FF catalyst exhibited the highest toluene degradation efficiency, CO 2 selectivity and O 3 decomposition capability. This plasma-Co/FF system significantly reduced the O 3 concentration from 112 ppm (plasma alone) to 26.2 ppm at a specific input energy (SIE) of 232 J/L. Density functional theory (DFT) calculations suggest that Co sites in CoFe 2 O 4 possess a lower O 3 adsorption energy and higher charge density potential to a higher oxygen vacancy formation tendency, promoting O 3 activation. This study provides an understanding of the mechanistic basis for the rational design of efficient plasma-catalytic systems for toluene removal.
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ANALYTICAL SCIENCES
·
2021
·Vol. 37
·期 2
·293-299
·
IF 2.081
Liu ZHANG,Yue HOU,Xiaoyan GUO,Wei LIU,Congcong LV,Xing PENG,Zixuan ZHANG
In this work, a new chemiluminescence (CL) system of Co-Fe prussian blue analogs nanocubes (Co-Fe PBA NCs) that can catalyze luminol to produce strong CL in the absence of H2O2 was established. Co-Fe PBA NCs have the property of oxidase-like activity, and it can catalyze the generation of active oxygen radicals in a dissolved oxygen system. Since caffeic acid (CA) can remove reactive oxygen species in the system, a sensitive detection method for CA on a paper-based chip was developed. Under the optimal conditions, this method showed a good linear response to CA in the range of 10 – 800 ng mL−1 with a limit of 3 ng mL−1. The proposed method had been used for the determination of CA in tea samples. The results may open a new avenue for the catalytic property on luminol CL system without extra oxidants.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Quanyun Ye,Jiayan Wu,Pingxiao Wu,Saeed Rehman,Zubair Ahmed,Nengwu Zhu
Efficient and low-cost catalysts for peroxymonosulfate (PMS) activation are needed for pollution prevention and environmental remediation. In this work, PMS activation by CoFe layered double hydroxide (CoFe-LDH) was promoted by compositing with biochar (BC). The characterization and catalytic performance of BC, CoFe-LDH, and BC@CoFe-LDH composite (BC-LDH) were investigated. The results indicated that BC could act as a catalyst carrier and electron mediator, which improved the physicochemical properties of CoFe-LDH and promoted the redox cycle of transition metals. The redox-active moieties (RAMs) of BC, especially the reduced functional groups (e.g., phenolic –OH), played an important role in the reduction of Co(III) and Fe(III). Remarkably, benefiting from the synergistic effect between BC and CoFe-LDH, the resulting BC-LDH exhibited excellent catalytic activity and stability for PMS activation. More reactive oxygen species (ROS) were produced in BC-LDH/PMS system. As a result, 100% of dimethyl phthalate (DMP, 10 mg L −1 ) degradation efficiency was achieved within 60 min in BC-LDH/PMS system, while only 62% in CoFe-LDH/PMS system. The intermediates of DMP degradation were identified and the degradation pathways were proposed. Our findings are expected to provide new insights into the rational design and application of BC materials and transition metals/PMS system for environmental remediation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Haofan Jia,Liujing Yang,Hao Zhu,Yang Wang,Ying Chen,Kai Sun,Xinbao Li
In this study, a series of high-efficient catalyst, Co–Fe/Al 2 O 3 , were synthesized via the sol-gel method for low-temperature phenol steam reforming (PSR). The optimized catalyst, 15Co–2Fe/Al 2 O 3 , exhibited a remarkable phenol conversion of 95.3%, a H 2 yield of 92.1% at 450 °C, GHSV = 7500 h −1 and a steam-to-carbon (S/C) ratio of 10. Furthermore, the catalyst activity was maintained for 660 min before a gradual decline was observed. The NH 3 -TPD analysis revealed that the addition of Fe enhanced the surface acidity of the catalyst, providing more active sites for phenol adsorption and activation. This study aims to address the challenges associated with high reaction temperatures and poor catalyst stability in PSR. Various characterization techniques have been employed to investigate the reaction mechanisms of bimetallic catalysts in low-temperature PSR.
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GREEN CHEMISTRY
·
2024
·Vol. 27
·期 1
·133-143
·
IF 9.3
Hongjiao Chen,Kewei Zhang,Yanzhi Xia,Jian Li,Bin Hui
Coupling the urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) in seawater is desirable to produce sustainable and green hydrogen due to the reduced energy consumption. However, developing high-performance UOR/HER electrocatalysts in seawater instead of pure water remains a great challenge. Herein, (B,P,Co,Fe)-Ni anchored on Paulownia Wood (PW) is proposed to enhance the overall urea-(sea)water splitting performance. The resulting sample only needs a potential of 1.34 V to deliver a large current density of 100 mA cm−2 for alkaline UOR and features a remarkable durability to maintain 100 mA cm−2 for 100 h. The HER and UOR (HER||UOR) coupled system in alkaline seawater-urea electrolyte for producing H2 demonstrated a more significantly reduced electrolyzer voltage of 1.67 V obtained at 100 mA cm−2 in comparison to that of the HER||OER system (1.98 V). The well-aligned micro-channels and nanopores in wood frameworks not only improve the hydrophilicity and aerophobicity of the whole electrode, which is conducive to the penetration of the electrolyte and release of bubbles, but also shorten the transmission distance of ions and intermediates to accelerate the reaction kinetic process. Density functional theory calculations reveal that Co, Fe, P and B co-doping in Ni effectively adjusts the electronic structure, and the adsorption/desorption behavior of the urea reaction intermediates is regulated by the synergistic effect from multiple components, resulting in an excellent catalytic activity in seawater-urea media. This work promotes a better understanding of the surface electronic structure modulation of nanowood via doping strategy and offers great potential in the design of advanced UOR/HER catalysts for hydrogen production and urea wastewater treatment.
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