Interface engineering of Ta[sub]3N[sub]5 thin film photoanode for highly efficient photoelectrochemical water splitting

Interface engineering is a proven strategy to improve the efficiency of thin film semiconductor based solar energy conversion devices. Ta3N5 thin film photoanode is a promising candidate for photoelectrochemical (PEC) water splitting. Yet, a concerted effort to engineer both the bottom and top interfaces of Ta3N5 thin film photoanode is still lacking. Here, we employ n-type In:GaN and p-type Mg:GaN to modify the bottom and top interfaces of Ta3N5 thin film photoanode, respectively. The obtained In:GaN/Ta3N5/Mg:GaN heterojunction photoanode shows enhanced bulk carrier separation capability and better injection efficiency at photo- anode/electrolyte interface, which lead to a record-high applied bias photon-to-current efficiency of 3.46% for Ta3N5-based photoanode. Furthermore, the roles of the In:GaN and Mg:GaN layers are distinguished through mechanistic studies. While the In:GaN layer con- tributes mainly to the enhanced bulk charge separation efficiency, the Mg:GaN layer improves the surface charge inject efficiency. This work demonstrates the crucial role of proper interface engineering for thin film-based photoanode in achieving efficient PEC water splitting

Components Interaction of Cotton Stalk under Low-Temperature Hydrothermal Conversion: A Bio-Oil Pyrolysis Behavior Perspective Analysis

The conversion of agricultural and forestry waste biomass materials into bio-oil by mild hydro-thermal technology has a positive effect on extending the agricultural industry chain and alleviating the world energy crisis. The interaction investigation of biomass components during bio-oil formation can be significant for the efficient conversion of lignocellulose when different raw materials are fed together. In this paper, a bio-oil pyrolysis behavior (thermogravimetric analysis, TG) perspective component interaction investigation of cotton stalks under low-temperature hydro-thermal conversion (220 °C) was studied. Cellulose, hemi-cellulose, lignin, and protein were used as lignocellulose model components, by their simple binary blending and multi-variate blending and combined with thermo-gravimetric analysis and gas chromatography-mass spectrometry (GC-MS) characterization and analysis. The interaction of different model components and real biomass raw material components in the hydro-thermal process was explored. Results showed that the components of hydro-thermal bio-oil from cotton stalks were highly correlated with the interactions between cellulose, hemi-cellulose, lignin, and protein. During the hydro-thermal process, cellulose and hemi-cellulose inhibit each other, which reduces the content of ketones, aldehydes, ethers, and alcohols in bio-oil. Interaction between cellulose and lignin was obvious, which promotes the formation of oligomers, such as ketones, aldehydes, esters, phenols, and aliphatic, while inhibiting the production of aromatic and multi-hybrid compounds. Otherwise, there was no obvious interaction effect between hemi-cellulose and lignin or between lignin and protein. This research will guide the industrialization of lignocellulose, especially the possible co-feed hydro-thermal conversion technology

Stable seawater oxidation with a self-healing oxygen-evolving catalyst

Direct seawater electrolysis is key to massive hydrogen fuel production without the depletion of precious freshwater resources and the need for high-purity electrolytes. However, the presence of high-concentration chloride ions (Cl−) and alkaline-earth metal ions (Mg2+, Ca2+) poses great challenges to the stability and selectivity of the catalysts for seawater splitting. Here, we demonstrate a self-healing oxygen evolution reaction (OER) catalyst for long-term seawater electrolysis. By suppressing the competitive chlorine evolution reaction and precipitating the alkaline-earth metal ions through an alkaline treatment of the seawater, stable seawater oxidation is achieved owing to the self-healing ability of the borate-intercalated nickel–cobalt–iron oxyhydroxides (NiCoFe-Bi) OER catalyst under highly-alkaline conditions. The self-healing NiCoFe-Bi catalyst achieves stable seawater oxidation at a large current density of 500 mA cm−2 for 1000 h with near unity Faraday efficiency. Our results have demonstrated strong durability and high OER selectivity of the self-healing catalyst under harsh conditions, paving the way for industrial large-scale seawater electrolysis

A self-healing catalyst for electrocatalytic and photoelectrochemical oxygen evolution in highly alkaline conditions.

While self-healing is considered a promising strategy to achieve long-term stability for oxygen evolution reaction (OER) catalysts, this strategy remains a challenge for OER catalysts working in highly alkaline conditions. The self-healing of the OER-active nickel iron layered double hydroxides (NiFe-LDH) has not been successful due to irreversible leaching of Fe catalytic centers. Here, we investigate the introduction of cobalt (Co) into the NiFe-LDH as a promoter for in situ Fe redeposition. An active borate-intercalated NiCoFe-LDH catalyst is synthesized using electrodeposition and shows no degradation after OER tests at 10 mA cm-2 at pH 14 for 1000 h, demonstrating its self-healing ability under harsh OER conditions. Importantly, the presence of both ferrous ions and borate ions in the electrolyte is found to be crucial to the catalyst's self-healing. Furthermore, the implementation of this catalyst in photoelectrochemical devices is demonstrated with an integrated silicon photoanode. The self-healing mechanism leads to a self-limiting catalyst thickness, which is ideal for integration with photoelectrodes since redeposition is not accompanied by increased parasitic light absorption

Topological Phase Transition-Induced Triaxial Vector Magnetoresistance in (Bi_1–<i>x</i>In_<i>x</i>)₂Se₃ Nanodevices

We report the study of a triaxial vector magnetoresistance (MR) in nonmagnetic (Bi_1–<i>x</i>In_<i>x</i>)₂Se₃ nanodevices at the composition of <i>x</i> = 0.08. We show a dumbbell-shaped in-plane negative MR up to room temperature as well as a large out-of-plane positive MR. MR at three directions is about in a −3%:–1%:225% ratio at 2 K. Through both the thickness and composition-dependent magnetotransport measurements, we show that the in-plane negative MR is due to the topological phase transition enhanced intersurface coupling near the topological critical point. Our devices suggest the great potential for room-temperature spintronic applications in, for example, vector magnetic sensors