Phase evolution of tantalum nitride and tantalum carbide films with PBII parameters

Tantalum nitride and tantalum carbide films were fabricated using magnetron sputtering of tantalum followed by nitrogen and carbon plasma-based ion implantation （N-PBII and C-PBII）. The phase evolution and morphology of the films were studied using glancing angle X-ray diffraction （GXRD） and transmission electron microscopy （TEM）. It was found that the main phase in the tantalum nitride films was crystalline TaNo.1 whose grain size increases with increasing implantation voltage and phase content increases with increasing implantation dose. In the tantalum carbide film, the main phase was Ta2C. TaC phase also appeared as the implantation dose increased. XRD results from various glancing angles show that the phases with high nitrogen or carbon content, Ta4N5 and TaC, are present in the surface of the films. X-ray photoelectron spectra （XPS） from the tantalum carbide film reveal that the surface carbon content is higher than that of the inner film.

Engineering tantalum nitride for efficient photoelectrochemical water splitting

Photoelectrochemical(PEC)water splitting is a promising energy conversion strategy for directly converting solar energy into green hydrogen fuel.Constructing an efficient PEC device,finding an efficient photoanode material with a suitable band gap and favorable band-edge positions is essential.Tantalum nitride(Ta_(3)N_(5))meets these fundamental requirements,and its theoretical maximum solar-to-hydrogen(STH)conversion efficiency can reach 15.9%.Consequently,it has been widely applied as a photoanode material for the PEC oxygen evolution reaction(OER).However,severe bulk and interface charge recombination,along with sluggish water oxygen kinetics,seriously limits its STH conversion efficiency for PEC water splitting.Herein,this feature article briefly reviews recent advances by our research group in improving the STH conversion efficiency of the Ta_(3)N_(5)photoanode using various strategies,including defect engineering,construction of a gradient band structure,interface engineering,and surface modification of self-healing OER cocatalyst.Up to now,the obtained half-cell STH efficiency has exceeded 4%,providing a solid foundation for the development of tandem PEC devices for unbiased solar-driven overall water splitting toward practical application.

Metal-seed assistant photodeposition of platinum over Ta_(3)N_(5) photocatalyst for promoted solar hydrogen production under visible light

Cocatalysts play a vital role in accelerating the reaction kinetics and improving the charge separation of photocatalysts for solar hydrogen production.The promotion of the photocatalytic activity largely relies on the loading approach of the cocatalysts.Herein,we introduce a metal-seed assistant photodeposition approach to load the hydrogen evolution cocatalyst of platinum onto the surface of Ta_(3)N_(5) photocatalyst,which exhibits about 3.6 times of higher photocatalytic proton reduction activity with respect to the corresponding impregnation or photodeposition loading.Based on our characterizations,the increscent contact area of the cocatalyst/semiconductor interface with metal-seed assistant photodeposition method is proposed to be responsible for the promoted charge separation as well as enhanced photocatalytic H2 evolution activity.It is interesting to note that this innovative deposition strategy can be easily extended to loading of platinum cocatalyst with other noble or non-noble metal seeds for promoted activities,demonstrating its good generality.Our work may provide an alternative way of depositing cocatalyst for better photocatalytic performances.

Effects of TaN nanoparticles on microstructure,mechanical properties and tribological performance of PEEK coating prepared by electrophoretic deposition

In order to solve the friction,wear and lubrication problems of titanium,a series of TaN/ployether−ether−ketone(PEEK)coatings were developed by electrophoretic deposition,and the effects of TaN nanoparticles on the microstructure,mechanical properties and tribological performance of coatings were explored.Results manifest that the introduction of TaN nanoparticles into PEEK coatings could improve the deposition efficiency,enhance the resistant deform capacity,increase the hardness,elastic modulus and adhesive bonding strength.Compared with the pure PEEK coating,the friction coefficient of P-TN-3 was greatly reduced by 31.25%.The wear resistance of P-TN-3 was also improved in huge boost,and its specific wear rate was decreased from 9.42×10^(−5) to 1.62×10^(−5) mm^(3)·N^(−1)·m^(−1).The homogeneous composite TaN/PEEK coatings prepared by electrophoretic deposition were well-adhered to the titanium alloy substrate,TaN nanoparticles could improve the strength of PEEK coating,and provide wear-resistance protection for titanium alloys.

Unravelling the essential difference between TiO_(x) and AlO_(x) interface layers on Ta_(3)N_(5) photoanode for photoelectrochemical water oxidation

Tantalum nitride(Ta_(3)N_(5))is a very promising photoanode material due to its narrow band gap(2.1 eV)and suitable band alignment for solar water splitting.However,it suffers from severe photocorrosion during water oxidation.In this work,it was found that surface passivation by AlO_(x) and TiO_(x) layers results in dramatically different PEC performance of Ta_(3)N_(5) photoanode for water oxidation.The mechanism study indicates that the negative charges on AlO_(x) can generate additional field to promote separation of photogenerated charges,while the positive charges on TiO_(x) layer show the opposite effect.As a result,the Ta_(3)N_(5) based photoanode modified with AlO_(x) layer gives a high photocurrent of 12.5 mA cm^(-2) for 24 h at 1.23 V versus the reversible hydrogen electrode(RHE).Dynamic analysis implies that the hole extraction and transfer are significantly improved by the modification with the AlO_(x) layer.This work reveals the importance of the charges on surface passivation layer in interface engineering of photoelectrodes.

Polysulfide regulation by defect-modulated Ta_(3)N_(5-x) electrocatalyst toward superior room-temperature sodium-sulfur batteries

Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nitride(Ta3N5-x)impregnated inside the interconnected nanopores of nitrogendecorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in roomtemperature sodium-sulfur batteries.Through a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of Ta3N5-x.The defect manipulation on the local environment enables well-regulated Ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of Ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide conversion.Moreover,the interconnected continuous Ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle behavior.Due to these attributes,the as-developed Ta3N5-x-based electrode achieves superior rate capability of 730 mAh g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mAh cm-2 under high sulfur loading of 6.2 mg cm-2.This work not only presents a new sulfur electrocatalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.