Search

In the quest for sustainable energy storage technologies, lithium‐based batteries, despite their prominence, face limitations such as high costs, safety risks, and supply chain issues. This has propelled the exploration of alternative materials, with aqueous aluminum‐ion batteries (AAIBs) emerging as a promising candidate due to their high energy density, abundance, and cost‐effectiveness. However, the low equilibrium reduction potential of aluminum ions presents significant challenges, including hydrogen evolution and poor cyclability. Addressing these, the study pioneers the application of single‐atom catalysts (SACs) in AAIBs, leveraging their high atom utilization and stability to enhance aluminum deposition and suppress hydrogen evolution. Sn, In, Cu, and Ni SACs are evaluated through density functional theory analysis and experimental validation, with Sn SAC identified as the most effective. Subsequently, the Sn SAC based anode demonstrates enhanced performance, achieving stable cycling over 500 h at 0.5 mA cm−2, significantly improved capacity retention (60 mAh g−1@300 cycles), and rate performance (50 mAh g−1@1 A g−1) in full cell tests. This work underscores the potential of SACs in advancing AAIB technology and opens new pathways for energy storage solutions. [ABSTRACT FROM AUTHOR]

Transition metal-nitrogen-carbon (M/NC) demonstrates a promising effective electrocatalyst for enhancing oxygen evolution/reduction reactions (OER/ORR). However, synthesizing these catalysts is often complex, time-consuming, and involves hazardous solvents while producing a low yield. This work introduces a versatile, eco-friendly, and straightforward solvent-free method to produce M/NC (M = Co, Ni, and Fe) catalysts in ~3 h using a glucose, urea, and metal nitrate hydrate mixture. The high-yield M/NC catalysts exhibit a porous architecture and uniform distribution of metal nanoparticles within a foaming flakes-like nitrogen-doped carbon matrix. The metal nanoparticles are wrapped with protective nitrogen-doped carbon layers, producing stable active sites. Possessing these unique properties, the obtained M/NC catalysts show high-performance and stable bifunctional OER/ORR. As the best result, Co/NC presents an OER/ORR potential difference (ΔE) of 0.78 V and retains 96% and 89% of its OER and ORR performance after a 10 h stability test. In practical application, the Co/NC-based Zn-air battery depicts a high power density of 184 mW cm-2 and good rechargeability of up to 120 h, outperforming the battery with noble metal-based catalysts. This work sheds light on the versatile, eco-friendly, and scalable synthesis of M/NC catalysts while presenting a strategy to accelerate the generation of inexpensive and highly effective bifunctional OER/ORR catalysts. [ABSTRACT FROM AUTHOR]

Discovering sources of transition metals, such as Ni, Co, and Mn, has become crucial due to their broad applicability, particularly as electrocatalysts for the oxygen evolution reaction (OER). Upcycled spent batteries have emerged as alternatives for transition metal sources for the OER electrocatalysts. In this work, Ni–Co–Mn oxalates were extracted from the spent LiNixCoyMnzO2 (NCM) cathode of lithium-ion batteries. The extracted oxalates were further processed via ball milling as a rapid and scalable mechanochemical route to engineer their structures. After calcination, Ni–Co–Mn oxides with nanosized granules on the surface that mainly consist of MnCo2O4 were obtained. With a correlation of morphology and trimetallic oxide formation with the OER catalytic performance, Ni–Co–Mn oxides exhibit OER overpotentials of 367 and 732 mV in alkaline and neutral media, respectively, showing OER catalytic activity in a wide pH range. The results indicate that ball milling can induce particle size reduction and bond formation between metals to facilitate mixed-metal oxide formation. Furthermore, the resulting material is also applicable as the catalyst in the air cathode of Zn-air batteries, where the battery achieved a power density of 85.42 mW cm–2 and 100 h of cycling stability, showing comparability with a battery with a Pt/C–Ir/C catalyst. [ABSTRACT FROM AUTHOR]

The silicon (Si) offers enormous theoretical capacity as a lithium‐ion battery (LIB) anode. However, the low charge mobility in Si particles hinders its application for high current loading. In this study, ball‐milled phosphorus‐doped Si nanoparticles encapsulated with nitrogen‐doped carbon (P−Si@N−C) are employed as an anode for LIBs. P‐doped Si nanoparticles are first obtained via ball‐milling and calcination of Si with phosphoric acid. N‐doped carbon encapsulation is then introduced via carbonization of the surfactant‐assisted polymerization of pyrrole monomer on P‐doped Si. While P dopant is required to support the stability at high current density, the encapsulation of Si particles with N‐doped carbon is influential in enhancing the overall Li+ diffusivity of the Si anode. The combined approaches improve the anode's Li+ diffusivity up to tenfold compared to the untreated anode. It leads to exceptional anode stability at a high current, retaining 87 % of its initial capacity under a large current rate of 4000 mA g−1. The full‐cell comprising P−Si@N−C anode and LiFePO4 cathode demonstrates 94 % capacity retention of its initial capacity after 100 cycles at 1 C. This study explores the effective strategies to improve Li+ diffusivity for high‐rate Si‐based anode. [ABSTRACT FROM AUTHOR]

Cation migration coupled with oxygen vacancy formation is known to drive the layered to disordered spinel/rock-salt phase transformation in the high-Ni layered oxide cathodes of Li-ion batteries. However, the effect of different electronic states of oxygen vacancies on the cation migration still remains elusive. Here, we investigate Ni migration in delithiated Ni-rich Li0.5Ni0.8Mn0.1Co0.1O2 (hence Li0.5NMC811) in the presence of neutral and charged oxygen vacancies by means of first-principles density functional theory (DFT) calculations coupled with the nudged elastic band (NEB) method. We find that oxygen vacancies with neutral or +2 charge favor the Ni migration to Li tetrahedral and/or octahedral sites, both thermodynamically and kinetically. As for the case of +1 charged oxygen vacancies, while they thermodynamicaly favor the Ni migration to the Li site, the relatively high migration barrier suggests that they kinetically prohibit the Ni migration. Our results suggest that controlling the formation of oxygen vacancies is the key to enhancing the Ni-rich NMC structural stability in particular in their charged states. [ABSTRACT FROM AUTHOR]

We study the effect of boron and sulfur doping on graphene with atomically dispersed zirconium as an electrocatalyst for the oxygen reduction reaction (ORR) by using density functional theory (DFT). The use of Zr as a metal center offers a highly stable catalyst due to the high electronegativity difference between Zr and its ligand. The origin of the ORR activity improvement has been investigated thoroughly. Here, we proposed a novel geometric descriptor for an atomically dispersed zirconium on a nitrogen-doped graphene catalyst with an axial oxygen ligand, which is the fractional coordination number of the Zr atom. We found that the fractional coordination number can successfully describe the shift of the dz2 band center in the doped compound, which is related to the binding energy of the Zr to the O ligand. We also found that the oxygen ligand is mobile during the adsorption process of ORR intermediates, and hence it is imperative for the axial oxygen ligand to bind neither too strongly nor too weakly to the Zr atom. The coordination engineering strategy can successfully enhance the ORR activity, shifting the ORR overpotential from 0.75 V and 0.92 V to 0.33 V and 0.32 V. This study provides new insights into the origin of ORR activity by connecting the novel geometric descriptor to the electronic structure and finally it is connected to the ORR activity. [ABSTRACT FROM AUTHOR]

Zn-air batteries (ZABs) with neutral electrolytes offer a significantly longer lifespan and better recyclability than alkaline ones. However, low-performance bifunctional catalytic activities for oxygen reduction or evolution reaction (i.e., ORR/OER) in neutral electrolytes still hamper their development. Here, we report iron nanoparticle-decorated nitrogen/boron co-doped reduced graphene oxide aerogel (Fe-NBrGO) with distinguished ORR/OER activity, enabling its application in neutral rechargeable ZABs. Taking advantage of the formation of 3D porous structure of graphene aerogel, N/B-moieties active sites, and Fe-containing active sites, Fe-NBrGO exhibits high ORR onset potential (1.074 and 0.817 V) and adequate OER overpotential (476 and 615 mV) in alkaline and neutral electrolytes, respectively. Fe-NBrGO enables the production of a neutral-ZAB with 34 mW cm−2 in peak power density and remains stable for a 284 h (~852 cycles) cycling test. This research highlights the rational design of highly active oxygen catalysts for the widespread implementation of new energy storage technologies. [ABSTRACT FROM AUTHOR]

The development of highly efficient separation membranes utilizing emerging materials with controllable pore size and minimized thickness could greatly enhance the broad applications of membrane-based technologies. Having this perspective, many studies on the incorporation of nanosheets in membrane fabrication have been conducted, and strong interest in this area has grown over the past decade. This article reviews the development of nanosheet membranes focusing on two-dimensional materials as a continuous phase, due to their promising properties, such as atomic or nanoscale thickness and large lateral dimensions, to achieve improved performance compared to their discontinuous counterparts. Material characteristics and strategies to process nanosheet materials into separation membranes are reviewed, followed by discussions on the membrane performances in diverse applications. The review concludes with a discussion of remaining challenges and future outlook for nanosheet membrane technologies. [ABSTRACT FROM AUTHOR]