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991.
Gang Liu Jingjing Li Chao Dong Liyuan Wu Dan Liang Huawei Cao Pengfei Lu 《International Journal of Hydrogen Energy》2021,46(35):18294-18304
Searching for the catalysts with excellent catalytic activity and high chemical stability is the key to achieve large-scale production of hydrogen (H2) through hydrogen evolution reaction (HER). Two-dimensional (2D) platinum and palladium dichalcogenides with extraordinary electrical properties have emerged as the potential candidate for HER catalysts. Here, chemical stability, HER electrocatalytic activity, and the origin of improved HER performance of Pt/Pd-based dichalcogenides with single-atom doping (B, C, N, P, Au, Ag, Cu, Co, Fe, Ni, Zn) and vacancies are explored by first-principles calculations. The calculated defect formation energy reveals that most defective structures are thermodynamically stable. Hydrogen evolution performance on basal plane is obviously improved by single-atoms doping and vacancies. Particularly, Zn-doped and Te vacancy PtTe2 have a ΔGH value close to zero. Moreover, defect engineering displays a different performance on HER catalytic activity in sulfur group elements, in order of S < Te < Se in Pd-based chalcogenides, and S < Se < Te in Pt-based chalcogenides. The origin of improved hydrogen evolution performance is revealed by electronic structure and charge transfer. Our findings of the highly activating defective systems provide a theoretical basis for HER applications of platinum and palladium dichalcogenides. 相似文献
992.
993.
Xilin Zhang Lu Chen Qian Sun Yudong Pang Xinwei Yang Zongxian Yang 《International Journal of Hydrogen Energy》2021,46(50):25457-25467
Modulating the surface electronic properties of the 2D MXenes is of significant importance to boost their hydrogen evolution reaction (HER) activity. Herein, a series of transition metal adatoms are employed to tune the surface electronic properties of Cr-based MXenes with oxygen function group for realizing impressive HER performance. The Results show that the charge of surface oxygen atoms, which is affected by both the host metal atoms and the adsorbed transition metal atoms, play critical role in the adsorption strength of hydrogen. The optimal performance is achieved by depositing Cr atom on the Cr2TiC2O2 MXene, which results in the adsorption free energy of hydrogen very close to zero (0.03 eV). Systematic electronic structure analyses confirm that the charge transfer from the adsorbed transition metals to the neighboring surface oxygen atoms could tune the orbital occupancy of oxygen and their adsorption strength to hydrogen atom and therefore the HER activity. These findings and concepts may be useful for the design of advanced MXene-based HER catalysts. 相似文献
994.
《International Journal of Hydrogen Energy》2021,46(74):36811-36823
Nitrogen-doped transition metal materials display promising potential as bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, Fe/N co-doped three-dimensional (3D) porous graphene (FeN-3D-PG) is prepared via a template method using sodium alginate as the carbon source and low polymerization degree melamine resin as the nitrogen source. The low polymerization degree melamine resin can form complexes with Fe3+ in the aqueous solution and further forms high density Fe-Nx active sites during pyrolysis. Meanwhile, the formed 3D porous structure efficiently promotes the uniform distribution of Fe-Nx active sites. The FeN-3D-PG catalyst exhibits pH-independent ORR activity. For OER, the catalyst possesses a low over potential (370 mV at 10 mA cm−2) in alkaline electrolyte. The Zn-air batteries (ZABs) using FeN-3D-PG as cathode exhibits a power density up to 212 mW cm−2, a high specific capacity of 651 mAh g−1, and the charge-discharge stability of 80 h. This work provides new sight to transition metal materials based ZABs with excellent performance. 相似文献
995.
996.
《Calphad》2021
Sodium hexatitanate (Na2Ti6O13) was reported as an anode side material for Sodium ion batteries owing to low material cost, high energy efficiency, good thermal stability and long cycle life. Therefore, studies pertaining to the thermodynamic properties of Na2Ti6O13 are indispensable for improving its service performance. However, a significant number of literature reviews concerning thermodynamic properties indicated that heat capacity of Na2Ti6O13 at high temperatures should be confirmed. In this study, the 99.5% purity of Na2Ti6O13 sample was successfully prepared via solid-state reaction using TiO2 and Na2CO3 as initial materials. Heat capacity of the as-synthesized samples in the temperature range of 573–1523 K was measured using a multi-high temperature calorimeter 96 line. Heat capacity, Cp, from 298.15 to 1573 K was modeled as a polynomial formula with a prediction error of 3%: Cp = 474.08143 + 0.06286T-8.04068 × 106 T−2 (J⋅mol−1⋅K−1). In combination with the low-temperature data, heat capacity of Na2Ti6O13 from 0 to 1573 K was given in present study. Values of changes in enthalpy, Gibbs free energy and entropy in the temperature range of 298.15–1573 K were calculated based on the temperature dependence of heat capacity. 相似文献
997.
Chia‐Che Chang Sin‐Ren Li Hung‐Lung Chou Yi‐Cheng Lee Shivaraj Patil Ying‐Sheng Lin Chun‐Chih Chang Yuan Jay Chang Di‐Yan Wang 《Small (Weinheim an der Bergstrasse, Germany)》2019,15(49)
The generation of ammonia, hydrogen production, and nitrogen purification are considered as energy intensive processes accompanied with large amounts of CO2 emission. An electrochemical method assisted by photoenergy is widely utilized for the chemical energy conversion. In this work, earth‐abundant iron pyrite (FeS2) nanocrystals grown on carbon fiber paper (FeS2/CFP) are found to be an electrochemical and photoactive catalyst for nitrogen reduction reaction under ambient temperature and pressure. The electrochemical results reveal that FeS2/CFP achieves a high Faradaic efficiency (FE) of ≈14.14% and NH3 yield rate of ≈0.096 µg min?1 at ?0.6 V versus RHE electrode in 0.25 m LiClO4. During the electrochemical catalytic reaction, the crystal structure of FeS2/CFP remains in the cubic pyrite phase, as analyzed by in situ X‐ray diffraction measurements. With near‐infrared laser irradiation (808 nm), the NH3 yield rate of the FeS2/CFP catalyst can be slightly improved to 0.1 µg min?1 with high FE of 14.57%. Furthermore, density functional theory calculations demonstrate that the N2 molecule has strong chemical adsorption energy on the iron atom of FeS2. Overall, iron pyrite‐based materials have proven to be a potential electrocatalyst with photoactive behavior for ammonia production in practical applications. 相似文献
998.
Interface reaction between alloys and submerged entry nozzle controlled by an electric current pulse
《Ceramics International》2021,47(20):28226-28236
To solve the limitations of clogging and erosion of the submerged entry nozzle (SEN) for the production of high-quality special steel, the chemical reactivity between different alloys and the SEN and the interface reaction between alloys and the SEN controlled by an electric current pulse (ECP) were examined in this study. Results revealed that the chemical reactivity between different alloys and the SEN is different. For example, the reactivity between rare-earth metal and the SEN was strong, while that between Al and the SEN was extremely weak. At the same time, some differences between the clogging and interface reaction by ECP control were observed. Typically, at the positive electrode of the SEN, when a stable and dense clogging layer is formed, the internal SEN was effectively protected. However, at the negative electrode of the SEN, the decarburization rate of the SEN was accelerated by ECP, probably leading to a vicious circle of accelerated clogging and erosion of the SEN. Therefore, in the future, issues of clogging, erosion, infiltration, and decarbonization between active alloys and the SEN in the casting process may be solved and regulated by using the positive electric field of ECP. Meanwhile, the gain effect of ECP also helped to promote the homogenization of molten steel. 相似文献
999.
《International Journal of Hydrogen Energy》2021,46(76):37977-37985
The poor kinetics is the main issue hindering MgH2 for practical hydrogen storage application. In this work, the tricarboxybenzene was used to construct the stable Ni MOF (Ni-BTC300) as the catalyst for MgH2. The prepared MOFs maintained their chemical structure after 300 °C calcining and doped to MgH2 by ball milling. The dispersed, uniformly bonded Ni atoms can improve the kinetics of the composites, which could desorb 5.14 wt% H2 within 3 min at 300 °C. And the stable MOF structure leading to good cycle stability in both kinetics and capacity, with retention of 98.2% after 10 cycles. 相似文献
1000.
A chemical reaction mode about GaN epitaxy in MOCVD is presented. We simulate the growth process of GaN in the vertical-spray MOCVD system on this mode using the KMC mothod. The result shows that adductive reaction mostly occurs at a lower temperature and pyrolytic reaction mostly occurs at a high temperature. And the growth rate increases with increasing temperature. This feature determines the surface morphology of the material. We also include the diffusion and desorption process of the reaction particle by the KMC method. These processes depend mostly on temperature and ultimately affect the surface morphology of the GaN material. 相似文献