Search

Rechargeable aqueous zinc‐ion batteries (ZIBs) with low cost and high safety arouse most promises as next‐generation energy storage configurations. Yet the heterogeneous electric field distributions and interfacial side reactions are considered stumbling roadblocks toward the commercialization of ZIBs. Here, these challenges via cationic electrostatic shielding and anionic preferential adsorption by sodium gluconate (SG) additive are addressed. The polar functional groups (─COO−) of SG anions preferentially anchor to the Zn anode, which can alter Zn2+ migration pathways and restrain side reactions. Moreover, as per the smaller effective reduction potential, the separated cations (Na+) from SG serve as a dynamic armor to provide strong electrostatic shielding effect for uniform Zn2+ deposition on the [002] crystal plane, radically eliminating Zn dendrite growth and promoting anti‐corrosion behaviors of Zn. Consequently, the Zn//Zn symmetric cell with modified electrolyte confers a lifespan of up to 600 h at a high 80% depth of discharge. Furthermore, even under a record‐low negative/positive ratio of 2.11 and lean electrolyte of 30 µL mAh−1, the Zn//VOX full cell remains enhanced capacity retention of 84.37% even after 800 cycles at 1 A g−1. This work develops an interfacial dual‐modulation strategy and provides unique insights to enlighten the practical application of ZIBs. [ABSTRACT FROM AUTHOR]

The development of lithium–sulfur (Li─S) batteries has been hampered by the shuttling effect of lithium polysulfides (LiPSs). An effective method to address this issue is to use an electrocatalyst to accelerate the catalytic conversion of LiPSs. In this study, heterogeneous MnP‐MnO2 nanoparticles are uniformly synthesized and embedded in porous carbon (MnP‐MnO2/C) as core catalysts to improve the reaction kinetics of LiPSs. In situ characterization and density functional theory (DFT) calculations confirm that the MnP‐MnO2 heterostructure undergo surface sulfidation during the charge/discharge process, forming the MnS2 phase. Surface sulfidation of the MnP‐MnO2 heterostructure catalyst significantly accelerated the SRR and Li2S activation, effectively inhibiting the LiPSs shuttling effect. Consequently, the MnP‐MnO2/C@S cathode achieves outstanding rate performance (10 C, 500 mAh g−1) and ultrahigh cycling stability (0.017% decay rate per cycle for 2000 cycles at 5 C). A pouch cell with MnP‐MnO2/C@S cathode delivers a high energy density of 429 Wh kg−1. This study may provide a new approach to investigating the surface sulfidation of electrocatalysts, which is valuable for advancing high‐energy‐density Li−S batteries. [ABSTRACT FROM AUTHOR]

Bi-based materials are promising catalysts for electrochemical reduction of carbon dioxide (CO2) to formate, but remain challenging in terms of activity and stability. Herein, we report the facile synthesis of Zn-doped Bi nanosheets (Zn–Bi NSs) as a highly active and robust catalyst for electrochemical reduction of CO2 to formate. Specifically, the Zn–Bi NS catalyst can be obtained using a hydrothermal method to prepare a Zn-decorated Bi2O2CO3 nanosheet followed by electrochemical reduction treatment. The as-prepared catalyst exhibits a remarkable formate faradaic efficiency of 94.6% and a high formate current density of 40.5 mA cm−2 at −1.2 V vs. reversible hydrogen electrode (RHE). In particular, the faradaic efficiency of formate remained at above 90% over a wide potential window from −0.8 to −1.2 V vs. RHE. In the H-type electrolytic cell, the Zn–Bi NS catalyst can be operated stably for 10 h at a cathode potential of −1.0 V vs. RHE with good retention of the physical phase. [ABSTRACT FROM AUTHOR]

Zn–CO2 batteries are excellent candidates for both electrical energy output and CO2 utilization, whereas the main challenge is to design electrocatalysts for electrocatalytic CO2 reduction reactions with high selectivity and low cost. Herein, the three‐phase heterojunction Cu‐based electrocatalyst (Cu/Cu2O‐Sb2O3‐15) is synthesized and evaluated for highly selective CO2 reduction to CO, which shows the highest faradaic efficiency of 96.3% at −1.3 V versus reversible hydrogen electrode, exceeding the previously reported best values for Cu‐based materials. In situ spectroscopy and theoretical analysis indicate that the Sb incorporation into the three‐phase heterojunction Cu/Cu2O‐Sb2O3‐15 nanomaterial promotes the formation of key *COOH intermediates compared with the normal Cu/Cu2O composites. Furthermore, the rechargeable aqueous Zn–CO2 battery assembled with Cu/Cu2O‐Sb2O3‐15 as the cathode harvests a peak power density of 3.01 mW cm−2 as well as outstanding cycling stability of 417 cycles. This research provides fresh perspectives for designing advanced cathodic electrocatalysts for rechargeable Zn–CO2 batteries with high‐efficient electricity output together with CO2 utilization. [ABSTRACT FROM AUTHOR]

The electrochemical performance of aqueous zinc metal batteries (AZMBs) is highly dependent on the electric double layer (EDL) properties at Zn electrode/electrolyte interface. Herein, a novel reconfigured EDL is constructed via a double‐charged theanine (TN) additive for super‐stable and deep‐rechargeable AZMBs. Experiments and theoretical computations unravel that the positively charged TN not only serves as preferential anchor to form a water‐poor Helmholtz plane onto the Zn anode, but also its anionic end could coordinate with Zn2+ to tailor the solvation structure in the diffusion layer and further reconstruct the inner H‐bonds networks, thus effectively guiding uniform Zn deposition and suppressing the water‐induced side reactions. Consequently, the Zn//Zn cells acquire outstanding cycling stabilities of nearly 800 h at a high depth of discharge of 80%. Moreover, the Zn//VOX full cells deliver substantial capacity retention (94.12% after 1400 cycles at 2 A g−1) under practical conditions. Importantly, the designed 2.7 Ah Zn//VOX pouch cell harvests a recorded energy density of 42.3 Wh Kgcell−1 and 79.5 Wh Lcell–1, with a remarkable capacity retention of 85.93% after 220 cycles at 50 mA g−1. This innovative design concept to reshape the EDL chemistry would inject fresh vitality into developing advanced AZMBs and beyond. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous Zn-ion batteries (ZIBs) have drawn incredible attention recently due to their high energy density, low cost, and intrinsic safety. However, water attacks that consistently corrode the Zn anode surface with the notorious dendrite growth, together with hydrogen evolution and inactive by-product formation seriously impede the practical applications of ZIBs. Here, we designed a bio-inspired electrolyte (DE) with a tetraethyl orthosilicate additive as a "healing agent" to repair the Zn surface wounds. The results revealed that the DE not only enabled an in situ formed zincophilic layer to promote the uniform Zn deposition, but also altered the Zn2+ solvation chemistry to suppress water-induced side reactions. Consequently, the Zn‖Zn cells with DE harvested an ultralong life of 6000 h at 0.5 mA cm−2 and 0.5 mA h cm−2 and 830 h even at a high depth of discharge of 80%. Furthermore, the Zn/V2O5 battery retained 93.15% of the initial capacity after 1000 cycles at 1 A g−1 with a low N/P ratio (2.0), lean electrolyte (20 μL mA h−1), and a high-capacity cathode (2.9 mA h cm−2). This work presents a fresh strategy for the development of high-performance ZIBs. [ABSTRACT FROM AUTHOR]