INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Lizi Chu,Yuan Lin,Yunpeng Liu,Hongjuan Wang,Qiao Zhang,Yuhang Li,Yonghai Cao,Hao Yu,Feng Peng
A facile method of loading CoS x nanosheet onto CdS nanorod has been designed, and the prepared CdS-CoS x composite catalyst exhibited significantly improved performance for photocatalytic hydrogen evolution compared with CdS catalyst. This composite catalyst was also used as a photoanode for photoelectrochemical (PEC) hydrogen production . The hydrogen production rate reached 168.6 μmol cm −2 h −1 (37.77 L m −2 h −1 ) under the simulated solar light, which is 2.7 times that of CdS and the same as that of CdS–Pt. In addition, in the Na 2 S–Na 2 SO 3 system for PEC hydrogen production, an abnormal relationship between photocurrent and the hydrogen production yield was found. By designing a series of experiments, the photocatalytic and photoelectrochemical characteristics for hydrogen production were reasonably revealed for the first time. In this work, the prepared structured catalyst is easy to be recycled, and CoS x can replace precious metal Pt, showing a promising application.
研究领域:
材料科学
·
能源科学
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Geying Liu,Chaoyue Xie,Yan Zhang,Ye Du,Jie Wang,Jia Lin,Jing Bai,Jinhua Li,Changhui Zhou,Tingsheng Zhou,Baoxue Zhou
Urea electrolysis is an appealing topic for hydrogen production due to its ability to extract hydrogen at a lower potential. However, it is plagued by sluggish kinetics and noble-metal catalyst requirements. Herein, we developed nickel-iron-layered double hydroxide (NiFe-LDH) nanolayers with abundant oxygen vacancies (O V ) via synergistically etching nickel foam with Fe 3+ and Cl - ions, enabling the efficient conversion of urea into H 2 and N 2 . The synthesized O V -NiFe-LDH exhibits a lower potential (1.30 vs. reversible hydrogen electrode, RHE) for achieving 10 mA cm −2 in the urea oxidation reaction (UOR), surpassing most recently reported Ni-based electrodes. O V provides favorable conductivity and a large surface area , which results in a 4.1-fold in electron transport and a 5.1-fold increase in catalyst reactive sites. Density Functional Theory (DFT) calculations indicate that O V can lower the adsorption energy of urea, and enhance the bonding strength of *CONHNH, giving rise to improved UOR. This study provides a viable path toward economical and efficient production of high-purity hydrogen.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 102
·84303-84310
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IF 3.84
Lian Duan,Yanling Chen,Kaixuan Zhang,Huoyan Luo,Jianxin Huang,Aihua Xu
The cobalt-based heterogeneous catalysts CoxOy-N/GAC were prepared by pyrolysis of a cobalt–phenanthroline complex on granular active carbon (GAC) in a nitrogen atmosphere, and tested for the degradation of Acid Orange 7 using hydrogen peroxide as a benign oxidant in a bicarbonate aqueous solution. Characterization by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and electron spin resonance spectroscopy revealed the formation of a cobalt oxide nanoparticle shell with a metallic Co core on the surface of GAC; and the nitrogen substituted the selected carbon atoms during the pyrolysis process and bonded to cobalt. The catalysts were active for dye decolorization in an aqueous solution containing 10 mM H2O2 and 5 mM NaHCO3 at room temperature. They also presented good stability with nearly no loss of cobalt ions after the reaction, in comparison with the high leaching of Co (0.25 mg L−1) from the CoxOy/GAC catalyst without nitrogen. The production of intermediates, the formation of reactive radicals and the effect of HCO3− were also investigated to further explore the efficiency of the catalyst. This study can provide a promising way for the activation of the green oxidant H2O2 in a bicarbonate aqueous solution by heterogeneous cobalt catalysts for environmental remediation.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Jialing Xu,Yawen Li,Xiaofen Chen,Guifang Li,Jiaqi Huo,Lishan Jia
Low-cost non-noble metal catalyst for dehydrogenation of formic acid to hydrogen at near room temperature is considered as a key to promoting commercial technology for clean energy. We have constructed reduced graphene oxide (RGO) self-assembly bonded nickel particles for synthesis of graphene nanosheets embedded with nickel nanoparticles architecture Ni@xRGO. Nitrogen and oxygen co-doped graphene facilitates the adsorption of hydrogen protons from formic acid. Electron transfer ability of Ni@xRGO with active sites is enhanced via Ni–C bond in the interface between the RGO nanosheets and nickel particles, which promoted the C–H bond breaking for dehydrogenation of formic acid. The Ni@0.20RGO has excellent catalytic performance for hydrogen production from formic acid at near room temperature (the yield of hydrogen, 240.0 mL g −1 h −1 at 50 °C), comparable to the most active non-noble metal catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Qingpo Peng,Xiuge Zhao,Manyu Chen,Jiajia Wang,Kai Cui,Xinjia Wei,Zhenshan Hou
The ionic materials consisting of cationic Ru complexes and Wells-Dawson polyoxometalate anion (POM, K 6 P 2 W 18 O 62 ) have been constructed via a non-covalent interaction. The as-synthesized catalysts have been characterized thoroughly by NMR, XRD, FESEM, and FT-IR, etc. The characterization suggested that a hydrogen bond interaction occurred between the proton of the amine ligand in the cationic Ru complexes and the oxygen atom of the POM anion. The hydrogen bond played an important role in enhancing catalytic activity for the transfer hydrogenation of methyl levulinate (ML) to γ-valerolactone (GVL) under very mild conditions. Especially, the transfer hydrogenation reaction proceeded via a heterogeneous catalysis approach and the heterogenized catalysts even afforded much better catalytic performance than homogeneous analogs. Notably, the catalysts can be recycled without an obvious loss of activity, and further extended to highly selective transfer hydrogenation of α,β-unsaturated ketones and aldehydes, etc. into the corresponding α,β-unsaturated alcohols without any base external additives. The high catalytic performance of these anchored catalysts was highly related to the hydrogen bond interaction and the basicity of the polyanion. The obtained knowledge from this work could lead us to a new catalysis concept of tethering active homogeneous complexes for constructing highly active anchored Ru complex catalysts for hydrogenation reaction.
研究领域:
催化化学
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材料科学
·
有机合成
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Jiachen Li,Qingwen Zhou,Zihan Shen,Shengwen Li,Jun Pu,Chenglin Zhong,Mengqiu Cao,Xin Jin,Huigang Zhang,Yaoyu Wang,Haixia Ma
Rational design of combined noble metals and earth abundant metal-based materials is important in the development of highly active and stable electrocatalysts with reduced noble metal loading toward hydrogen evolution reaction (HER). As a cheaper alternative to platinum (Pt), ruthenium (Ru) has similar bond strength with hydrogen. In this work, we develop carbon fiber-supported cobalt carbonate hydroxides nanowires for the deposition of Ru (CF@Ru–CoCH NWs) and achieve high HER performance under alkaline condition. Such novel catalyst exhibits a low Tafel slope (65 mV dec −1 ), small overpotential of, respectively, 66 and 121 mV at geometrical current density of −10 and −100 mA cm −2 . The superior performance, comparable to commercial Pt for HER, is attributed to the synergistic effect from Ru nanoparticles (NPs) and cobalt carbonate hydroxides nanowires (CoCH NWs). Dual-pathway kinetic analysis confirms that the CoCH NWs are able to lower the energy barrier of the Volmer step while Ru improves the Heyrovsky step to form hydrogen gas, thereby enhancing overall HER activity.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Yutong Li,Tianyi Dai,Quanxuan Wu,Xingyou Lang,Lijun Zhao,Qing Jiang
NiFe layered double hydroxide (LDH)-based materials arouse great attention because of their outstanding catalytic activity for oxygen evolution reaction (OER) under alkaline conditions. However, its catalytic activity for hydrogen evolution reaction (HER) under alkaline conditions is relatively poor. Herein, to improve the HER catalytic activity of NiFe LDH under alkaline conditions, we design a heterostructure of NiS and NiS 2 on NiFe LDH and successfully achieve Mo element doping . The catalyst named NiFe-LDH@Mo–NiS–NiS 2 /NF possesses a three-dimensional nano-flower-like structure and shows an outstanding catalytic performance for both HER and OER. Specifically, in 1 M KOH solution, it requires the low overpotentials of 261 and 120 mV to achieve the current density of 50 and 10 mA cm −2 for OER and HER, respectively. Simultaneously, when NiFe-LDH@Mo–NiS 2 –NiS/NF is used as the bifunctional catalysts, it only needs a low voltage of 1.63 V to achieve a current density of 10 mA cm −2 . The outstanding catalytic performance is attributed to its special heterostructure and the synergy between Mo and NiS x , resulting in comparability with most reported non-noble metal-based catalysts. The doping of metal elements and the construction of heterostructures provide new ideas for the structure regulation and performance improvement of bifunctional electrocatalysts .
研究领域:
材料科学
·
电催化
✓ 已验证
DOI
高影响因子
Catalysts
·
2016
·Vol. 6
·期 9
·134
·
IF 2.964
Songbai Qiu,Ying Xu,Yujing Weng,Longlong Ma,Tiejun Wang
A series of MCM-41 supported Ni catalysts with high metal dispersion was successfully synthesized by simple co-impregnation using proper ethylene glycol (EG). The acquired Ni-based catalysts performed the outstanding hydrogenolysis activity of guaiacol. The effects of the synthesis parameters including drying temperature, calcination temperature, and metal loading on the physical properties of NiO nanoparticles were investigated through the use of X-ray diffraction (XRD). The drying temperature was found to significantly influence the particle sizes of NiO supported on MCM-41, but the calcination temperature and metal loading had less influence. Interestingly, the small particle size (≤3.3 nm) and the high dispersion of NiO particles were also obtained for co-impregnation on the mixed support (MCM-41:HZSM-5 = 1:1), similar to that on the single MCM-41 support, leading to excellent hydrogenation activity at low temperature. The guaiacol conversion could reach 97.9% at 150 °C, and the catalytic activity was comparative with that of noble metal catalysts. The hydrodeoxygenation (HDO) performance was also promoted by the introduction of acidic HZSM-5 zeolite and an 84.1% yield of cyclohexane at 240 °C was achieved. These findings demonstrate potential applications for the future in promoting and improving industrial catalyst performance.
研究领域:
催化化学
·
能源化学
·
材料化学
·
工业催化
·
生物质转化
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2017
·Vol. 46
·期 32
·10620-10629
·
IF 4.029
Songsong Li,Dongsheng Dai,Lei Ge,Yangqin Gao,Changcun Han,Nan Xiao
Novel layer-like Ni(OH)2 co-catalyst-decorated ZnIn2S4 microsphere photocatalysts were synthesized for the first time via a facile in situ deposition method to boost the photocatalytic H2-production performance. The physical and optical properties of the as-prepared Ni(OH)2–ZnIn2S4 composite samples were characterized via X-ray diffraction (XRD), transmission electron microscopy (TEM), UV-vis diffusion reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and surface photovoltage spectroscopy (SPV). The results indicate that the photocatalytic H2 evolution activity of the ZnIn2S4 microspheres under visible light irradiation significantly enhances by introducing inexpensive Ni(OH)2 as a co-catalyst. The 5 mol% Ni(OH)2–ZnIn2S4 sample shows the highest H2-production rate of 8.35 mmol g−1 h−1, which is 18 times higher than that of pure ZnIn2S4. Moreover, photocatalytic activity of the Ni(OH)2–ZnIn2S4 sample remains stable even after 4 cycling photocatalytic experiments. In addition, a possible mechanism on the enhanced photocatalytic activity was proposed and verified by surface photovoltage spectroscopy.
研究领域:
材料科学
·
光催化
·
能源化学
·
纳米材料
·
半导体催化
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Mantang Chen,Zhimin Zhang,Lihua Zhu,Nan Wang,Heqing Tang
The present work aimed at using bisulfites (HSO 3 − ) to enhance the oxidative degradation of bisphenol A (BPA) in a Fenton process based on the Fe 3+ -H 2 O 2 reagents. It was confirmed that both the degradation and mineralization of BPA were drastically enhanced by the addition of HSO 3 − . Typically, the use of 0.1 mmol L −1 Fe 3+ , 0.3 mmol L −1 HSO 3 − and 10 mmol L −1 H 2 O 2 achieved a complete degradation of BPA (0.05 mmol L −1 ) in only 2 min. The addition of HSO 3 − increased the BPA degradation rate constant from 0.045 min −1 in the Fe 3+ -H 2 O 2 system to 2.71 min −1 in the Fe 3+ -HSO 3 − -H 2 O 2 system by 60 times. This drastic enhancement effect of HSO 3 − was attributed to its complexing and reducing abilities. The formation of FeSO 3 + complex prevented the precipitation of Fe 3+ and accelerated the cycling of Fe 3+ /Fe 2+ ; the reducing ability of HSO 3 − further favored the transformation of Fe 3+ to Fe 2+ . Several reactive species, including OH, SO 3 − and SO 4 − were responsible for the degradation of BPA, among which OH was the dominant one. The proposed Fe 3+ -HSO 3 − -H 2 O 2 system is suggested be able to act as the followed stage of a traditional Fe 2+ -H 2 O 2 system in the engineering setting.
研究领域:
环境科学
·
化学工程
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2020
·
IF 3.594
Huisi Yang,Juan Zhou,Jing Bao,Yi Ma,Jun Zhou,Caihong Shen,Huibo Luo,Mei Yang,Changjun Hou,Danqun Huo
Hydrogen peroxide (H 2 O 2 ) is an important intermediate in biological and environmental systems, which is widely used in pharmaceutical, environmental protection, fuel cell and other fields. It is also the most important signal conducting molecule, second messenger and growth factor in Reactive Oxygen Species (ROS). The increase of intracellular H 2 O 2 level is closely related to cancer and neurodegenerative diseases. Therefore, the detection of H 2 O 2 is an important goal of clinical research. Herein, we synthesized molybdenum disulfide (MoS 2 ) with a lattice spacing of 0.62 nm using a simple method, maintaining the excellent characteristics of MoS 2 itself, and performing sensitive detection of H 2 O 2 . In this work, we use graphene oxide as the precursor, and use one-step hydrothermal method to synthesize three-dimensional molybdenum disulfide/reduced graphene oxide composite (MoS 2 /rGO). Graphene not only provides a support structure for the growth of MoS 2 , but also forms large number of pores in it. These channels greatly increase the specific surface area of the MoS 2 /rGO composite and provide a sufficient reaction environment for the reaction of H 2 O 2 on the composite. Its greatly improves the sensitivity of the MoS 2 /rGO enzyme-free sensor. We have calculated that the enzyme-free sensor composed of this electrode has a good linear dependence on the H 2 O 2 concentration in the range of 2 μM to 23.18 mM, and the detection limit is 0.19 μM. The enzyme-free sensor with simple preparation method is expected to be greatly developed in the clinical application of hydrogen peroxide sensor.
研究领域:
分析化学
·
生物医学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jun Zhang,Songying Qu,Bing Li,Xiaoyan Li,Lin Lin
The practical use of Fenton process has been thus far limited by the harsh pH and accumulation of iron-rich sludge, while these two shortcomings will be tackled hopefully via developing non-metallic-catalyzed green Fenton-like approach. Herein, we investigate in-situ the dynamic evolution of electrode surface atomic hydrogen (H*) and H* mediated pH-independent and residue-free electro-Fenton process via operando electrochemical investigation and visualization techniques. The H* generated on the surface of palladium-coated electrode enables effective activation of hydrogen peroxide (H 2 O 2 ) to generate hydroxyl radical ( OH) for efficient bisphenol A degradation (>99%), validated by in-situ cyclic voltammetry and electron spin resonance. Meanwhile, in-situ Raman spectra confirms that H 2 O 2 is activated through a transition state of *H 3 O 2 adduct with a low reaction energy barrier of 0.51 eV, whereby the lone electron in H* can readily cleave peroxide bond to produce OH and H 2 O as the only products ( ΔG = −1.03 eV). More importantly, the electron-driven H* production is independent of the solution pH as both H + and H 2 O can act as precursors verified by in-situ fluorescence analyses, so that the H 2 O 2 activation mediated by H* extends successfully to a wider pH range (3–10). Our research provides a promising path toward eliminating restrictions of traditional Fenton process and paves the way simultaneously for in-situ investigation into reaction mechanism of such electrochemical processes.
研究领域:
环境科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）