Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H2O2). In this work, we theoretically and experimentally discovered that atomically dispersed Lewis acid sites (octahedral M–O species, M = aluminum (Al), gallium (Ga)) regulate the electronic structure of adjacent carbon catalyst sites. Density functional theory calculation predicts that the octahedral M–O with strong Lewis acidity regulates the electronic distribution of the adjacent carbon site and thus optimizes the adsorption and desorption strength of reaction intermediate (*OOH). Experimentally, the optimal catalyst (oxygen-rich carbon with atomically dispersed Al, denoted as O-C(Al)) with the strongest Lewis acidity exhibited excellent onset potential (0.822 and 0.526 V versus reversible hydrogen electrode at 0.1 mA cm−2 H2O2 current in alkaline and neutral media, respectively) and high H2O2 selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H2O2 production.
Engineering the morphology and electronic properties simultaneously of emerging metallene materials is an effective strategy for enhancing their performance as oxygen reduction reaction (ORR) electrocatalysts. Herein, a highly efficient and stable ORR electrocatalyst, Fe-doped ultrathin porous Pd metallene (Fe–Pd UPM) composed of a few layers of 2D atomic metallene layers, was synthesized using a simple one pot wet-chemical method and characterized. Fe–Pd UPM was measured to have enhanced ORR activity compared to undoped Pd metallene. Fe–Pd UPM exhibits a mass activity of 0.736 A mgPd –1 with a loss of mass activity of only 5.1% after 10 000 cycles at 0.9 V versus the reversible hydrogen electrode (vs RHE) in 0.1 M KOH solution. Density functional theory (DFT) calculations reveal that the stable Fe dopant in the inner atomic layers of Fe–Pd UPM delivers a much smaller overpotential during O* hydrogenation into OH*. The morphology, porous structure, and Fe doping were verified to have enhanced ORR activity. We believe that the rational design of metallene materials with porous structures and interlayer doping is promising for the development of efficient and stable electrocatalysts.
CsPbI2Br perovskite solar cells (PSCs) based on carbon electrodes (CEs) are considered to be low-cost and thermally stable devices. Nevertheless, the insufficient contact and energy level mismatch between the CsPbI2Br layer and CE hinder the further enhancement of the cell efficiency. Herein, a carbon black (CB) interlayer was introduced between the perovskite layer and CE. The hole extraction was facilitated due to the larger contact area and suitable energy band alignment in the CsPbI2Br/CB interface. Further investigation indicated the diffusion of CB nanoparticles from the CE or CB layer to the CsPbI2Br film after a certain period of time. We disclosed the formation of a CB-CsPbI2Br bulk heterojunction structure due to the carbon diffusion, which resulted in an efficiency enhancement. As a result, a record efficiency of 13.13% is achieved for carbon-based inorganic PSCs. This work also reveals that the diffusion of CB nanoparticles in CB-containing PSCs is universal and inevitable, although this kind of diffusion results in the enhancement of cell efficiency.
The development of highly efficient non‐precious metal electrocatalysts for the oxygen evolution reaction (OER) in low‐grade or saline water is currently of great importance for the large‐scale production of hydrogen. In this study, by using an electrochemical activation pretreatment, metal oxy(hydroxide) nanosheet structures derived from self‐supported nickel–iron phosphide and nitride nanoarrays grown on Ni foam are successfully fabricated for OER catalysis in saline water. It is demonstrated that the different NiOOH and NiOOH@FeOOH (NiOOH grown on FeOOH) structures are generated from nickel–iron nitride and phosphide, respectively, after electrochemical activation. In particular, the NiOOH@FeOOH heteroarchitecture shows outstanding electrocatalytic performance with an ultralow overpotential of 292 mV to drive the current density of 500 mA cm−2. An unconventional dual‐sites mechanism (UDSM) is proposed to address the OER process on NiOOH@FeOOH and show that the FeOOH underlayer plays a critical role regarding the enhanced OER activity of NiOOH. The new possible UDSM involving two reaction sites presents a different understanding of the OER process on multi‐OH layer complexes, which is expected to guide the design of heteroarchitecture electrocatalysts.
Thermoplastic polyamide elastomers (TPAEs) have emerged as important thermoplastic elastomer materials with significant potentials owing to their excellent low‐temperature flexibility, easy processability, lightweight, good thermal stability and mechanical properties, etc. Over the last few decades, TPAEs have rapidly developed into a large variety of kinds of TPAEs. Striking advancements have been achieved in this research field. Unfortunately, there is not yet a review to summarize the progress. The present paper summarizes the major advancements dealing with TPAEs, in which synthesis, structures/properties as well as applications are introduced in detail. Moreover, current challenges and main developmental directions dealing with TPAEs are also presented. This review may motivate more interest in TPAEs, further facilitating their all‐side research and more large‐scale applications.
Fast and stable production of hydrogen peroxide (H 2 O 2 ) through electrochemical pathways is crucial for wastewater treatment applications. With this objective, herein, we report an integrated and superaerophilic electrode composed of atomically dispersed Ni−O−C site-enriched carbon nanosheets (IS-NiOC electrode) for electrochemical oxygen reduction to produce H 2 O 2 . Both experimental and theoretical results have proven that atomically dispersed Ni−O−C sites enable a low overpotential (260 mV at 0.1 mA cm −2 ) and high selectivity (>90% at 0.0−0.5 V vs reversible hydrogen electrode (RHE)) in a neutral electrolyte. Compared with a commercial gas-diffusion electrode, the IS-NiOC electrode offers stronger affinity to oxygen bubbles and more robust three-phase contact points, resulting in high current density (∼106 mA cm −2 at 0.25 V vs RHE) and superior stability (∼200 h). These merits allow the application of the IS-NiOC electrode in an electro-Fenton-like process, which enables fast degradation of representative organic pollutants in both a steady state and a flow state.
A small amount of ruthenium (Ru) was introduced into binary CoSe 2 /C through chemical reduction to obtain ternary Ru(CoSe 2 )/C. The effects of heat-treatment (HT) on crystal structures and electrocatalytic activities toward oxygen reduction reaction (ORR) of binary and ternary catalysts were investigated. Upon the heat-treatment at 400 • C, a simple phase transformation from orthorhombic to cubic CoSe 2 took place in the absence of Ru, resulting in larger crystallite size and poorer ORR activity of CoSe 2 /C-HT. However, with the incorporation of Ru, a new cubic (Ru x Co y )Se 2 like phase might be formed as the Ru could enter the CoSe 2 lattice during the phase transformation, which not only prevented the grain growth and stabilized the structure, but also provided the new efficient ORR active site. Ultimately, high activity and excellent stability were achieved for Ru(CoSe 2 )/C-HT with the synergy of Ru with Co and Se, which significantly enhanced Ru utilization. The open circuit potential and maximum power density reached 0.87 V and 151 mW • cm −2 in the H 2 /O 2 single cell test, respectively, which were 24.3% and 242.5 times larger than those of CoSe 2 /C-HT (0.70 V and 0.62 mW • cm −2 ), respectively. The normalized degradation was 2.2% after 1000 cycles during the accelerated degradation test.
Lead halide perovskites have emerged as promising photovoltaic (PV) materials owing to their superior optoelectronic properties. However, they suffer from poor stability and potential toxicity. Here, computational screening with experimental synthesis is combined to explore stable, lead-free, and defect-tolerant PV materials. Heavy cations with lone-pair electrons and mixed anions of chalcogens and halogens as a descriptor for simultaneous realization of defect tolerance and high stability are adopted. Together with the criteria of possessing direct band gap and optimal gap value, the inorganic material database is screened and CuBiSCl 2 in the post-perovskite structure is identified with an ideal band gap of 1.37 eV. The electronic structure and defect calculations suggest its defect-tolerant characteristics. By optical absorption measurement, its band gap is confirmed to be ≈1.44 eV, with strong absorption near the band edge. The material is stable against thermal decomposition up to 300 °C and can survive from 25 days of storage at ambient conditions with 60% relative humidity. Prototype solar cells are fabricated and demonstrate an open circuit voltage of 1.09 V and a power conversion efficiency of 1.00%. With the excellent properties above, CuBiSCl 2 is proposed to be a promising candidate for PV application.
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