Highly active sites of low spin FeⅡN4species:The identification and the ORR performance

Over recent years,catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction(ORR).However,the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being obtained.Herein Fe₃C/C and Fe₂N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15%CH₄/H₂and pure NH₃,respectively.By acid leaching of Fe₂N/C sample,only single sites of FeN₄species were presented,providing an ideal model for identification of catalytic functions of the single sites of FeN₄in ORR.A correlation was conducted between the concentration of Fe^ⅡN₄in low spin state by Mossbauer spectra and the kinetic current density at 0.8 V in alkaline media,and such a structure-performance correlation assures the catalytic roles of low spin Fe^ⅡN₄ species as highly active sites for the ORR.     

Enhanced photo-electrochemical activity of ZnO/Cu2S nanotube arrays photocathodes

ZnO/Cu₂S nanotube arrays are fabricated firstly by a facile and capping-agent-free method, and the photo-electrochemical performance has been studied systematically. The results show that ZnO/Cu₂S nanotube arrays achieve enhanced photo-electrochemical water splitting performance and the photocurrent densities of ZnO/Cu₂S are 7.9 times than that of ZnO at 0 V versus Ag/AgCl. The performance of the ZnO/Cu₂S nanotube arrays can be adjusted by changing the amount of Cu₂S microcrystals. The results confirm that the enhanced photo-electrochemical performance of ZnO/Cu₂S is due to the significantly improved visible light absorption, effective separation of photo-induced carriers due to the well band energy match and the formed p-n junction between ZnO and Cu₂S.     

Insights into low-carbon hydrogen production methods: Green,blue and aqua hydrogen

The primary aim of this study is to provide insights into different low-carbon hydrogen production methods. Low-carbon hydrogen includes green hydrogen (hydrogen from renewable electricity), blue hydrogen (hydrogen from fossil fuels with CO₂ emissions reduced by the use of Carbon Capture Use and Storage) and aqua hydrogen (hydrogen from fossil fuels via the new technology). Green hydrogen is an expensive strategy compared to fossil-based hydrogen. Blue hydrogen has some attractive features, but the CCUS technology is high cost and blue hydrogen is not inherently carbon free. Therefore, engineering scientists have been focusing on developing other low-cost and low-carbon hydrogen technology. A new economical technology to extract hydrogen from oil sands (natural bitumen) and oil fields with very low cost and without carbon emissions has been developed and commercialized in Western Canada. Aqua hydrogen is a term we have coined for production of hydrogen from this new hydrogen production technology. Aqua is a color halfway between green and blue and thus represents a form of hydrogen production that does not emit CO₂, like green hydrogen, yet is produced from fossil fuel energy, like blue hydrogen. Unlike CCUS, blue hydrogen, which is clearly compensatory with respect to carbon emissions as it captures, uses and stores produced CO₂, the new production method is transformative in that it does not emit CO₂ in the first place. In order to promote the development of the low-carbon hydrogen economy, the current challenges, future directions and policy recommendations of low-carbon hydrogen production methods including green hydrogen, blue hydrogen, and aqua hydrogen are investigated in the paper.     

In situ Raman spectroscopic study towards the growth and excellent HER catalysis of Ni/Ni(OH)2 heterostructure

The electrochemical water splitting to produce H₂ in high efficiency with earth-abundant-metal catalysts remains a challenge. Here, we describe a simple “cyclic voltammetry + ageing” protocol at room temperature to activate Ni electrode (AC-Ni/NF) for hydrogen evolution reaction (HER), by which Ni/Ni(OH)₂ heterostructure is formed at the surface. In situ Raman spectroscopy reveals the gradual growth of Ni/Ni(OH)₂ heterostructure during the first 30 min of the aging treatment and combined with polarization measurements, it suggests a positive relation between the Ni/Ni(OH)₂ amount and HER performance of the electrode. The obtained AC-Ni/NF catalyst, with plentiful Ni–Ni(OH)₂ interfaces, exhibits remarkable performance towards HER, with the low overpotential of only 30 mV at a H₂-evolving current density of 10 mA/cm² and 153 mV at 100 mA/cm², as well as a small Tafel slope of 46.8 mV/dec in 1 M KOH electrolyte at ambient temperature. The excellent HER performance of the AC-Ni/NF could be maintained for at least 24 h without obvious decay. Ex situ experiments and in situ electrochemical-Raman spectroscopy along with density functional theory (DFT) calculations reveal that Ni/Ni(OH)₂ heterostructure, although partially reduced, can still persist during HER catalysis and it is the Ni–Ni(OH)₂ interface reducing the energy barrier of H1 adsorption thus promoting the HER performance.     

渣油催化临氢热转化钼铁双金属催化剂的研究

Replacement of precious single metal catalysts with cost-effective, highly-dispersed composite catalysts for catalytic hydrothermal conversion of residue holds tremendous promise for the residue upgrading technologies. Organic metals were added to the feed as the oil-soluble precursors, and transformed into the catalytic active phases in this work. Physical properties and structures of the composite catalysts had been investigated by X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, scanning electron microscope and transmission electron microscopy. The composite catalysts were found to be highly efficient in the catalytic hydrothermal conversion of both model compound and residue. Increased metal dispersion and synergistic effects of two metals played indispensable roles in such catalytic system. Results showed that under the test conditions in the article, the catalyst had the best catalytic performance when the mass ratio of molybdenum to iron was 1.5.     

Controlled Secure Direct Communication Protocol via the Three-Qubit Partially Entangled Set of States

In this paper, we first re-examine the previous protocol of controlled quantum secure direct communication of Zhang et al.’s scheme, which was found insecure under two kinds of attacks, fake entangled particles attack and disentanglement attack. Then, by changing the party of the preparation of cluster states and using unitary operations, we present an improved protocol which can avoid these two kinds of attacks. Moreover, the protocol is proposed using the three-qubit partially entangled set of states. It is more efficient by only using three particles rather than four or even more to transmit one bit secret information. Given our using state is much easier to prepare for multiqubit states and our protocol needs less measurement resource, it makes this protocol more convenient from an applied point of view.     

High-rate capability of carbon-coated micron-sized hexagonal TT-Nb2O5 composites for lithium-ion battery

With excellent specific capacity, superior cycle stability, safety and strong practical, Nb₂O₅ has been considered as one of the prospective anode materials for lithium-ion batteries (LIBs). However, current study suggests that Nb₂O₅ electrode materials for LIBs still face the vital issues of low electrical conductivity and poor rate performance. Therefore, carbon-coated TT-Nb₂O₅ materials are designed and synthesized through solid state method in this work, which present high specific capacity (228 mA h g^?1 at 0.2C), satisfactory rate properties (107 mA h g^?1 at 20 C). The outstanding electrochemical property can not only give the credit to the pseudocapacitance effect of TT-Nb₂O₅, but also attribute to introduction of carbon. The homogeneous carbon-coated materials enhance the electrical conductivity, increase the electron transmission speed and alleviate particle crushing. This research not only offers a new method for preparing excellent electrode materials, but also provides a kind of excellent anode material with prospective application for LIBs.