Development of cost-effective and efficient electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of prime importance to emerging renewable energy technologies. Here, we report a simple and effective strategy for enhancing ORR and OER electrocatalytic activity in alkaline solution by introducing Asite cation deficiency in LaFeO 3 perovskite; the enhancement effect is more pronounced for the OER than the ORR. Among the A-site cation deficient perovskites studied, La 0.95 FeO 3-δ (L0.95F) demonstrates the highest ORR and OER activity and, hence, the best bifunctionality. The dramatic enhancement is attributed to the creation of surface oxygen vacancies and a small amount of Fe 4+ species. This work highlights the importance of tuning cation deficiency in perovskites as an effective strategy for enhancing ORR and OER activity for applications in various oxygen-based energy storage and conversion processes.
We demonstrate that the electronic devices built on patterned graphene nanoribbons (GNRs) can be made with atomic-perfect-interface junctions and controlled doping via manipulation of edge terminations. Using first-principles transport calculations, we show that the GNR field effect transistors can achieve high performance levels similar to those made from single-walled carbon nanotubes, with ON/OFF ratios on the order of 10(3)-10(4), subthreshold swing of 60 meV per decade, and transconductance of 9.5 x 10(3) Sm-1.
As a highly appealing technology for hydrogen generation, water electrolysis including oxygen evolution reaction (OER) at the anode and hydrogen evolution reaction (HER) at the cathode largely depends on the availability of efficient electrocatalysts. Accordingly, over the past years, much effort has been made to develop various electrocatalysts with superior performance and reduced cost. Among them, ruthenium (Ru)-based materials for OER and HER are very promising because of their prominent catalytic activity, pH-universal application, the cheapest price among the precious metal family, and so on. Herein, recent advances in this hot research field are comprehensively reviewed. A general description about water splitting is presented to understand the reaction mechanism and proposed scaling relations toward activities, and key stability issues for Ru-based materials are further given. Subsequently, various Ru-involving electrocatalysts are introduced and classified into different groups for improving or optimizing electrocatalytic properties, with a special focus on several significant bifunctional electrocatalysts along with a simulated water electrolyzer. Finally, a perspective on the existing challenges and future progress of Ru-based catalysts toward OER and HER is provided. The main aim here is to shed some light on the design and construction of emerging catalysts for energy storage and conversion technologies.
Layered LiCo0.8 Fe0.2 O2 demonstrates dramatically enhanced oxygen evolution reaction (OER) activity and durability in an alkaline solution over LiCoO2 and other reported state-of-the-art catalysts, including benchmark IrO2 . This superior performance is attributed to Fe-doping-induced synergistic effects.
Perovskite oxide is an attractive low-cost alternative catalyst for oxygen evolution reaction (OER) relative to the precious metal oxide-based electrocatalysts (IrO and RuO). In this work, a series of Sr-doped La-based perovskite oxide catalysts with compositions of LaSr FeO ( x = 0, 0.2, 0.5, 0.8, and 1) are synthesized and characterized. The OER-specific activities in alkaline solution increase in the order of LaFeO (LF), LaSrFeO (LSF-0.2), LaSrFeO (LSF-0.5), SrFeO (SF), and LaSrFeO (LSF-0.8). We establish a direct correlation between the enhancement in the specific activity and the amount of surface oxygen vacancies as well as the surface Fe oxidation states. The improved specific activity for LSF-0.8 is clearly linked to the optimum amount of surface oxygen vacancies and surface Fe oxidation states. We also find that the OER performance stability is a function of the crystal structure and the deviation in the surface La and/or Sr composition(s) from their bulk stoichiometric compositions. The cubic structure and lower deviation, as is the case for LSF-0.8, led to a higher OER performance stability. These surface performance relations provide a promising guideline for constructing efficient water oxidation.
The self‐catalyzed growth of nanostructures on material surfaces is one of the most time‐ and cost‐effective ways to design multifunctional catalysts for a wide range of applications. Herein, the use of this technique to develop a multicomponent composite catalyst with CoSx core encapsulated in an ultrathin porous carbon shell entangled with Co, N‐codoped carbon nanotubes is reported. The as‐prepared catalyst has a superior catalytic activity for oxygen evolution and oxygen reduction reactions, an ultralow potential gap of 0.74 V, and outstanding durability, surpassing most previous reports. Such superiority is ascribed, in part, to the unique 3D electrode architecture of the composite, which is favorable for transporting oxygen species and electrons and creates a synergy between the components with different functionalities. Moreover, the flexible solid Zn–air battery assembled with such an air electrode shows a steady discharge voltage plateau of 1.25 V and a round‐trip efficiency of 70% at 1 mA cm−2. This work presents a simple strategy to design highly efficient bifunctional oxygen electrocatalysts and may pave the way for the practical application of these materials in many energy conversion/storage devices.
To date, various stretchable conductors have been fabricated, but simultaneous realization of the transparency, high stretchability, electrical conductivity, self-healing capability, and sensing property through a simple, fast, cost-efficient approach is still challenging. Here, α-lipoic acid (LA), a naturally small biological molecule found in humans and animals, is used to fabricate transparent (>85%), electrical conductivity, highly stretchable (strain up to 1100%), and rehealable (mechanical healing efficiency of 86%, electrical healing efficiency of 96%) ionic conductor by solvent-free one-step polymerization. Furthermore, the ionic conductors with appealing sensitivity can be served as strain sensors to detect and distinguish various human activities. Notably, this ionic conductor can be fully recycled and reprocessed into new ionic conductors or adhesives by a direct heating process, which offers a promising prospect in great reduction of electronic wastes that have brought acute environmental pollution. In consideration of the extremely facile preparation process, biological available materials, satisfactory functionalities, and full recyclability, the emergence of LA-based ionic conductors is believed to open up a new avenue for developing sustainable and wearable electronic devices in the future.features. [1][2][3][4] These conductors provide huge opportunities for promising applications of artificial muscles, skin sensors, biological actuators, stretchable displays, electronic eye cameras, intelligent robot arms, and others. [5][6][7][8][9][10][11] It was well known that the conventional electronic conductors are normally prepared from waferbased materials, which possess several drawbacks including fragility, rigidity, and low conductivity under large-scale deformations. [12] They cannot satisfy the demands of high stretchability, flexibility, durability, and stability. To achieve these criteria, strain engineering and nanocomposites are the two most adoptable strategies to fabricate stretchable conductors. In the first strategy, nonstretchable inorganic materials, such as silicon and metals, are geometrically patterned into buckled, serpentine structures on elastomeric substrates that renders the conductors excellent sensitivity and larger workable range of strain. [10,13,14] Nonetheless, most resultant conductors still show narrow range of strain from 20% to 70%, [15] and presents out-of-plane patterns that is difficult to encapsulate. Meanwhile, this strategy usually involves expensive and very complicated techniques, which greatly limits the further development of these conductors. Integrating conductive fillers into polymer matrix to produce nanocomposites used as stretchable conductors is the second strategy. [16] So far, various nanomaterials, such as carbon nanotubes, [17][18][19][20] carbon black, [21] graphene-based materials, [22,23] metal nanowires, and nanoparticles, [24,25] have been used as conductive fillers because of their unique mechanical and electrical properties. Although the robu...
Although metallic ruthenium (Ru) is a potential electrocatalyst for the hydrogen evolution reaction (HER) to replace platinum (Pt) at a cost of only ≈4% of Pt, the persistent dissolution of Ru under operation conditions remains a challenge. Here, it is reported that agglomerates of large ruthenium phosphide (RuP) particles (L-RP, ≈32 nm) show outstanding HER performance in pH-universal electrolytes, which particularly demonstrates a surprisingly higher intrinsic activity and durability than small nanoparticles of RuP (S-RP, ≈3 nm) or metallic Ru on carbon supports. This is especially true in basic media, achieving electrocatalytic activity comparable to or even outperforming that of Pt/C, as reflected by lower overpotential at 10 mA cm , smaller Tafel slope, larger exchange current density, and higher turnover frequency while maintaining 200 h stable operation. Calculations suggest that ΔG of RuP is much closer to zero than that of metallic Ru, and phosphorous doping is proven to enhance the rate of proton transfer in HER, contributing in part to the improved activity of RuP. The better performance of L-RP than that of S-RP is ascribed largely to the stabilization of the P species due to the lowered surface energy of large particles. Furthermore, the relatively low-cost materials and facile synthesis make L-RP/C a highly attractive next-generation HER electrocatalyst.
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