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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Coupling ultralow-content ruthenium with nickel hydroxide via corrosion engineering for highly efficient hydrogen generation from ammonia borane

Yang Luo,Yao Tian,Shiyu Yang,Jing Jiang,Aike Liu,Hejun Gao,Lunhong Ai

Efficient and controllable release of hydrogen from solid hydrogen storage materials is a promising way to produce hydrogen safely and on-demand. The development of economical, highly active, easily recyclable catalysts is critical for practical applications, which remains a great challenging. Herein, the easily controllable and cost-effective corrosion strategy is ingeniously developed to simply prepare ultralow-content ruthenium coupled with nickel hydroxide on nickel foam (Ru–Ni–NF). After experiencing the spontaneous oxidation-reduction reactions between the reactive NF and Ru 3+ , ultrafine Ru nanoparticles decorated nickel hydroxide nanosheets are in situ intimately grown on porous NF networks. The optimal Ru–Ni–NF catalyst exhibits the excellent performance for catalytic hydrolysis of ammonia borane with a high turnover frequency (TOF) of 539.6 mol H2 mol Ru −1 min −1 at 298 K and a low apparent activation energy of 36.4 kJ mol −1 , due to the synergistic effect between Ru nanoparticles and nickel hydroxide nanosheets. Furthermore, the Ru–Ni–NF catalyst possesses easy separation and outstanding durability, which is superior to powdered catalysts. This study provides a facile and economical strategy for the preparation of ultralow-content noble metal supported metal foam-type catalysts for dehydrogenation of ammonia borane.

研究领域: 材料科学 · 催化化学
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Effects of Manganese Doping into Nickel Hydroxides for the Electrochemical Conversion of KA Oil

Jie Chen,Yi Shen

Selective oxidative cleavage of C(OH)–C or C(O)–C bonds in cyclohexanol and cyclohexanone (KA oil) to produce adipic acid (AA), a monomer for the synthesis of nylon-66, is of significant importance for the petrochemical industry. Herein, we report an electrochemical method to improve the efficiency for upgrading KA oil into AA. Free-standing electrodes consisting of hydroxides (Ni(OH)2 and Mn-doped Ni(OH)2) supported by carbon paper were fabricated via an in situ electrodeposition process and further examined for KA oil conversion. The morphology and structures of the samples were characterized by field emission scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and Raman spectroscopy. The electrochemical performance of the samples was studied by cyclic voltammetry, linear sweep voltammetry, and electrochemical impedance spectroscopy. The products of KA oil oxidation were analyzed by high-performance liquid chromatography. The introduction of manganese into nickel hydroxides enhanced the catalytic performance in terms of activity and product selectivity. Specifically, the optimal sample exhibited a current density of 50 mA mg–1 and selectivity of 46.8%, which are superior to those of pure nickel hydroxides. Such enhancement was attributed to the electronic interaction of manganese with nickel hydroxides, thereby modifying the adsorption of the substrates. Interestingly, the introduction of Mn into nickel hydroxides had negligible effects in the oxygen evolution reaction. The effects of critical parameters including substrate composition, reaction temperatures, KOH concentrations, and electrolysis time on the conversion of KA oil were investigated.

CAS / MDL: 110-94-1
研究领域: 材料科学 · 电化学 · 催化反应
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Catalysts · 2020 ·Vol. 10 ·期 2 ·189 · IF 3.52

A Novel Reduced Graphene Oxide-Attapulgite (RGO-ATP) Supported Fe2O3 Catalyst for Heterogeneous Fenton-like Oxidation of Ciprofloxacin: Degradation Mechanism and Pathway

Ting Zhang,Chunyuan Qian,Pengran Guo,Shuchai Gan,Lingyu Dong,Ge Bai,Qiyang Guo

Ciprofloxacin, a third-generation fluoroquinolones (FQs) antibiotic, is observed to increasingly pollute the environment. In this study, a three-dimensional reduced graphene oxide-attapulgite-based catalyst Fe2O3/RGO-ATP was prepared and used to analyze the degradation of ciprofloxacin in a heterogeneous Fenton reaction. The heterogeneous catalyst Fe2O3/RGO-ATP was prepared by a one-step hydrothermal method, and the samples were characterized using BET(Brunauer-Emmett-Teller) surface area, Raman spectroscopy, X-ray diffraction (XRD), Fourier infrared (FTIR) spectroscopy, scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The effect of reaction time, temperature, pH, initial concentration, H2O2dosage and reuse time on the degradation of ciprofloxacin by the catalyst Fe2O3/RGO-ATP was investigated. The optimum conditions of degradation of ciprofloxacin are observed to be 60 °C, pH 5, H2O2concentration of 2.9724 mmol/L, and initial ciprofloxacin concentration of 50 mg/L. The catalyst could be reused several times with a decline in catalytic capacity. Fourier-transform ion cyclotron resonance mass spectrometer (FT) was also employed to study the degradation products of ciprofloxacin in the aqueous solution. The results show that the heterogeneous catalyst Fe2O3/RGO-ATP possessed an excellent ability for the catalytic degradation of ciprofloxacin. Direct hydroxyl oxidation is noted to be the main pathway of degradation of ciprofloxacin, and no defluorination reaction is observed during the degradation process.Keywords:graphene;ciprofloxacin;catalytic degradation;hydroxyl oxidation

CAS / MDL: 85721-33-1 7782-42-5
研究领域: 环境科学 · 材料科学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2023 ·Vol. 170 ·期 1 ·017503 · IF 3.9

Dual-Signal Colorimetric and Electrochemical Sensor of Dopamine Based on Nanocomposite of Cobalt Oxyhydroxide/Carbon Black

Xun Zou,Zilong Deng,Huiting Chen,Zhiyuan Zheng,Limin Ji,Yuying Chen,Mingyan Sun,Sixue Ouyang,Zhiying Yuan,Peng Zhao,Jia Tao

In this report, a novel electrochemical and colorimetric dual-mode sensing system was developed for the sensitive and selective detection of DA. The large surface area of CoOOH and the excellent conductivity of CB endow the electrochemical sensing system with high sensitivity. CoOOH with oxidase-like activity will convert the colorless TMB into the blue oxidation product OXTMB, appearing an absorption peak at 652 nm correspondingly. And the addition of DA will inhibit the activity of oxidase followed by a reducing in the absorption. Our device provided a wider detection range for DA from 1 to 30 μM and 1 to 950 μM through colorimetric and electrochemical methods, respectively. Furthermore, this biosensor with good biocompatibility has been successfully used for in-vitro tracking of DA efflux from live PC12 cell after being stimulated, which has important scientific and practical value for clinical diagnosis and monitoring.

研究领域: 生物传感 · 分析化学 · 神经科学
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INORGANIC CHEMISTRY · 2023 · IF 4.6

Regulating Complex Transition Metal Oxyhydroxides Using Ni3S2: 3D NiCoFe(oxy)hydroxide/Ni3S2/Ni Foam for an Efficient Alkaline Oxygen Evolution Reaction

Yating Fan,Weidong Shi,Longhua Li

In electrochemical decomposition of water, the slow kinetics of the anodic oxygen evolution reaction (OER) is a challenge for efficient hydrogen production. Heterointerface engineering is a desirable way to rationally design electrocatalysts for the OER. Herein, we designed and fabricated a nanoparticle flower-like NiCoFe(oxy)hydroxide catalyst in situ grown on the surface of Ni3S2/NF to construct a heterojunction via combining hydrothermal and electrodeposition methods. The heterostructure exhibits a smaller overpotential of 254 mV at a large current density of 100 mA cm–2 in 1 M KOH than that of pristine NiCoFeOxHy/NF (356 mV) and Ni3S2/NF (471 mV). Tafel and electrochemical impedance spectroscopy further showed a favorable kinetics during electrolysis. The role of the substrate Ni3S2 was explored via density functional theory calculations. Our calculations found that SOx on the Ni3S2 surface is a strong nucleophilic group and the synergy effect between Fe and SOx could break *OOH to reduce the Gibbs energy. We also found that the contribution of SOx in sulfates to the OER activity could be negligible. Furthermore, a series of comparative samples were prepared to test this synergy effect. Our experiments indicated that the introduction of Ni3S2 is beneficial. The present contribution provides an important helpful insight into the design and fabrication of novel and highly efficient heterostructure electrocatalysts by introducing nucleophilic groups at the interface.

CAS / MDL: 12125-01-8
研究领域: 材料科学 · 电化学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Synthesis of ferrihydrite/polyaniline composite using waste Fe(III)/EPS-cultures with polyaniline and its application for tetracycline photo-Fenton degradation

Shuyue Wang,Dan Hu,Yang Liu,Huixin Xiong

Antibiotics pollutants are arousing seriously environmental issues, so the highly efficient photo-Fenton catalysts have been developed in their treatments. In this work, according to the results of XRD, Raman, FTIR, and XPS, ferrihydrite/polyaniline (Fh/PANI) catalyst could be successfully prepared in waste iron-bacterial cultures (shorted as Fe(III)/EPS-solutions) with PANI conductor ((C 6 H 7 N) n , 200–300 nm). The Fh/PANI was an optimal photo-Fenton catalyst with good physical properties for tetracycline hydrochloride (TCH, C 22 H 25 ClN 2 O 8 ) degradation. In photo-Fenton systems with 30 mmol/L H 2 O 2 , 40 mg/L TCH, 0.2 g/L catalyst, and pH 4.0 under the visible light irradiation, degradation efficiency was 94% for Fh/PANI (82% for Fh). Kinetics data of TCH degradation well followed to pseudo-first-order model ( R 2 =0.974 for Fh/PANI, and R 2 =0.929 for Fh). The Fh/PANI catalyst had a good stability for TCH degradation, and the efficiencies ranged in 94%−77% within its five runs. The TCH could be efficiently mineralized into H 2 O and CO 2 inorganic molecules, and the producing ∙O 2 − was the key action group. These results indicate Fh/PANI photo-Fenton catalyst will have a potential application in treating antibiotic polluted waters. It also can provide a good approach of preparing Fe-(oxyhydr)oxide/conductor composites in waste iron-bacterial cultures.

CAS / MDL: 64-75-5
研究领域: 环境科学 · 生物化学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

The mechanism for promoted oxygenation of V(IV) by goethite: Positive effect of surface hydroxyl groups

Xingyun Hu,Xianjia Peng,Linghao Kong,Feng Zhu

The most toxic and mobile form of vanadium (V) is V(V). Thus, the oxidation of V is a subject of considerable importance since the process may increase environmental risks of V. V(IV) is known to be stable when pH < 4.5. However, in this study, stable V(IV) was oxidized almost completely in goethite suspension within 60 min at pH 2.0 and pH 4.0, correspondingly, only 25%–30% and 15%–20% of V(IV) were oxidized in equimolar Fe 3+ solution and the blank solution, respectively. The promoted oxidation of V(IV) by FeOOH is attributed to the formation of the complex, VO(OFe<) + or VO(OFe<) 2 . On the one hand, the formation of the complex caused higher pH in the interface of solid FeOOH and corresponding lower conditional potential of V(V)/V(IV) than those in bulk solutions, which facilitates the oxidation of V(IV). On the other hand, the surface group OFe < may serve as a medium that facilitating the electron transfer from V(IV) ions to dissolved oxygen molecules, also favoring the oxidation of V(IV). This study not only deepens our understanding of the transfer, transformation, and risk of V in environments, but also provides a reference to speculate the fate of similar elements in environments.

研究领域: 环境化学 · 地球化学 · 水污染控制 · 金属形态转化 · 界面过程
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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Novel Cobalt Germanium Hydroxide for Electrochemical Water Oxidation

Zhe Xu,Wenchao Li,Xiaohui Wang,Bing Wang,Zhan Shi,Cheng Dong,Shicheng Yan,Zhigang Zou

Developing efficient and stable oxygen evolution catalyst (OEC) is a critical step to overcome the sluggish kinetics of water oxidation. Here, we hydrothermally synthesized a novel OEC, cobalt germanium hydroxide, CoGeO2(OH)2. The inherent Co-bonded hydroxyl groups facilitate the formation of active oxygen evolution reaction intermediates. Meanwhile, the facile leaching of Ge at the OEC–electrolyte interface contributes to surface reconstruction, generating Co-based (oxy)hydroxides, which would weaken its lattice constraint and suppress the excessive corrosion in the OEC bulk. As a result, CoGeO2(OH)2 reveals good catalytic activity and stability. This CoGe-based OEC achieves the overpotential at 10 mA cm–2 (η@10mA) of ∼340 mV, and the turnover frequency of ∼0.08 s–1. And the electrolysis kept at ∼10 mA cm–2 could be sustained for over 350 h. In addition, this p-type CoGeO2(OH)2 is demonstrated to be an effective electrocatalytic overlayer on n-type Ta3N5 photoanode, remarkably decreasing the onset for nearly 400 mV and increasing the photocurrent density at 1.23 VRHE about 3.8 times.

研究领域: 材料科学 · 电化学
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FIRE SAFETY JOURNAL · 2022 · IF 3.78

Extinguishing capability of novel ultra-fine dry chemical agents loaded with iron hydroxide oxide

Haoran Jiang,Yong Jiang,Rujia Fan

This study aimed to develop high-efficiency fire extinguishing agents that is halogen-free and phosphorus-free, natural clinoptilolite (CP) was used as a carrier to adsorb iron, and iron-loaded functional clinoptilolite (ICP) was prepared. The structure and morphology of the samples were characterized by Fourier transform infrared spectrometer , X-ray diffractometer, X-ray photoelectron spectroscopy, and scanning electron microscopy. The results showed that a layer of FeOOH is attached to the surface of the functionalized ICP, forming elliptical particles with a length of 100–500 nm, and the iron content can reach 4.99%. The suppression experiment involving pool fires indicated that the fire extinguishing performance of ICP is better than CP and commercial ABC dry powders fire extinguishing agents. The average extinguishing time and usage of ICP were reduced by 41.4% and 40.1%, respectively, compared with ABC powders. The improvement of the fire-extinguishing performance of ICP was mainly since the loaded iron ions are converted into active iron atoms during high-temperature combustion and participate in the catalytic reaction of capturing combustion radicals.

CAS / MDL: 7647-01-0
研究领域: 材料科学 · 消防工程
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Sustainable Energy & Fuels · 2021 ·Vol. 5 ·期 8 ·2228-2233 · IF 6.367

Efficient water oxidation using flower-like multiphase nickel hydroxide with Fe doping

Xinyue Zhang,Yanling Qiu,Wenxiu Zhang,Xuqiang Ji,Jingquan Liu

Ingeniously designing a water-oxidation catalyst with advantages of a large surface area, multicomponent synergy, and optimized electronic structure, especially utilizing a one-step reaction system to achieve these dominant characteristics is pivotal to high-performance electrochemical water splitting. Here, flower-like multiphase nickel hydroxide catalysts doped with Fe (Fe-α,β-Ni(OH)2) are fabricated through a one-pot solvothermal-coordination methodology. The resulting Fe-α,β-Ni(OH)2 presents excellent oxygen production activity. An overpotential of 267 mV is required to drive a current density of 30 mA cm−2. Fe-α,β-Ni(OH)2 achieves stable operation for over 20 h. The considerable OER performance should result from the unique bionic flower structure, large surface area, and Fe-doping as well as the unique phase interfaces between the α- and β-Ni(OH)2 components. Our study provides a new trial of combining several favorable structural features into one material system that benefits efficient OER catalysis based on earth-abundant Fe and Ni elements.

研究领域: 材料科学 · 电化学 · 催化科学
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Synthesis of Al-modified hydrochar from corn stover for efficient phosphate removal

E. Shuang,Qiong Wang,Kuichuan Sheng,Ximing Zhang

The development of a simple and feasible process for preparing adsorbent materials to recover phosphorus resources would have significant environmental and social benefits. In this study, the Al-modified hydrochar was synthesized for phosphate adsorption by hydrothermal carbonization in one pot using corn stover as raw material. The results showed that phosphate adsorption mainly depended on the precipitation reaction between Al element and phosphate, in which the hydrochar carrier played a synergistic role. Al element through the hydrothermal treatment loaded on hydrochar expressed a much higher phosphate adsorption performance than that on pyrochar. When the concentration of AlCl 3 solution added in the hydrothermal process was 2 mol·L −1 and the hydrothermal temperature exceeded 180 ℃, Al element could transform from the amorphous state, which was less effective for phosphate adsorption, to Al 24 O 11 (OH) 44 Cl 6 crystal with high adsorption performance and could be more stably loaded onto the hydrochar. Although the preparation process was simple, the adsorption performance of hydrochar is good. The phosphate adsorption capacity and removal efficiency by the hydrochar prepared at 260 °C reached to 114.40 mg·g −1 and 76.27%, which could be further increased by adjusting the dosage of adsorbent and pH of water. The pseudo-second-order kinetic model and Langmuir isotherm model could better describe the phosphate adsorption process on Al-loaded hydrochar. Phosphate was rapidly adsorbed on the surface of the hydrochar rich in mesoporous structure and bound to the surface-active sites. This study could transform agricultural waste into a functional hydrochar-based adsorbent and provide a low-cost, simple operation and efficient phosphate removal technology .

CAS / MDL: 7784-13-6 7778-77-0
研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

In-situ growth and electronic structure modulation of urchin-like Ni–Fe oxyhydroxide on nickel foam as robust bifunctional catalysts for overall water splitting

Zixia Wan,Hongbo Yu,Qiuting He,Yan Hu,Puxuan Yan,Xue Shao,Tayirjan Taylor Isimjan,Bing Zhang,Xiulin Yang

The rational design of non-precious-metal bifunctional catalysts of oxygen and hydrogen evolution reactions that generate a high current density and stability at low over potentials is of great significance in the field of water electrolysis. Herein, we report a facile and controllable method for the in-situ growth of urchin-like FeOOH–NiOOH catalyst on Ni foam (FeOOH–NiOOH/NF). X-ray photoelectron spectroscopy confirms that the proportion of Ni and Fe species with high valence state gradually increase with the extension of growth time. Electrochemical studies have shown that the optimized FeOOH–NiOOH/NF-24 h and −12 h catalysts demonstrate excellent electrochemical activity and stability in oxygen/hydrogen evolution reactions. Moreover, the cell voltage is reduced around 0.15 V at high current density (0.5–1.0 A cm −2 ) as compared to the state-of the art RuO 2 /NF(+)||Pt–C/NF(−) system, far better than most of the previously reported catalysts. The cost analyst revealed that using FeOOH–NiOOH/NF catalyst as both electrodes could potentially reduce the price of H 2 around 7% compared with traditional industrial electrolyzers. These excellent electrocatalytic properties can be attributed to the unique urchin-like structure and the synergy between Ni and Fe species, which can not only provide more active sites and accelerate electron transfer , but also promote electrolyte transport and gas emission.

研究领域: 材料科学 · 电化学
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