Correction for 'Regulating Zn2+/H+ selectivity through functional group design of separators for long-lifespan aqueous zinc batteries' by Jiaxian Zheng et al., Mater. Horiz., 2025, https://doi.org/10.1039/d5mh00358j.

Zn anodes in aqueous rechargeable zinc batteries (AZBs) are plagued by irreversibility issues stemming from dendrite growth, hydrogen evolution, and corrosion. The design of separator offers a promising approach to enhance the reversibility of Zn anodes, but a universal strategy for rational separator design remains elusive. In this study, we propose a comprehensive design principle that takes into account the selective binding with Zn2+, H+ and H2O, and further suggest that separators should ideally exhibit strong binding strength with H+ and H2O but weak with Zn2+. We explore four typical scenarios based on varying binding strengths and identify polyethersulfone (PES) as a highly promising separator through screening of various commercial separators. Both experiment and theoretical calculations reveal that PES effectively regulates the transfer of Zn2+, H+ and H2O, thereby concurrently suppressing dendrite growth, hydrogen evolution, and corrosion. As a result, the Zn‖Zn symmetric battery can operate for over 4000 h at 1 mA cm-2 and 1 mA h cm-2. Furthermore, the full battery can deliver an impressive lifespan of over 6400 cycles at 3 A g-1. This work not only introduces a new separator for high-performance AZBs but also provides guiding principles for functional separator design.

Electrochemical nitrate reduction reaction (NO 3 RR) towards ammonia, as an emerging and appealing technology alternative to the energy-intensive Haber–Bosch process and inefficient nitrogen reduction reaction, has recently aroused wide concern and research. However, the current research of the NO 3 RR towards ammonia lacks the overall performance comparison of various electrocatalysts. Given this, we here make a comparison of 12 common transition metal oxide catalysts for the NO 3 RR under a high cathodic current density of 0.25 A·cm −2 , wherein Co 3 O 4 catalyst displays the highest ammonia Faradaic efficiency (85.15%) and moderate activity (ca. −0.25 V vs. reversible hydrogen electrode). Other external factors, such as nitrate concentrations in the electrolyte and applied potential ranges, have also been specifically investigated for the NO 3 RR.

The sustainable development of catalysts with Pt-like catalytic activity to produce hydrogen economically from water electrolysis is essential and challenging. Herein, we have prepared a novel catalyst with the combined virtues of nanocolumn structures and heterojunctions by magnetron sputtering molybdenum nitride (Mo2N) thin films over cobalt-metal-organic framework (Co-MOF) nanocolumns on carbon paper (CP), and explored the catalytic activities in hydrogen evolution reaction (HER). By optimizing the preparation process, the heterostructured Co-MOF@Mo2N/CP catalysts can exhibit an excellent HER performance with an overpotential of only 72.8 mV at 10 mA cm-2 and cycling durability over 24 h and 5000 cycles, achieving one of the best performances among state-of-the-art Mo-based catalysts. This work guides and accelerates the design of low-cost and high-performance transition metal nitrides HER catalysts for industrial applications.

Transition metal nitrides (TMNs) are rapidly gaining prominence as attractive supercapacitor electrode materials due to their intriguing properties. Nevertheless, the quest for facile and green fabrication of TMNs electrodes with high supercapacitor performance remains a substantial challenge. In this study, we have successfully designed and prepared the binder-free V-doped CrN thin film electrodes through a one-step reactive magnetron co-sputtering in nitrogen and argon atmosphere without high temperature heating. Our experimental and DFT findings confirm that the V doping increases the number of active sites, enlarges the specific surface area, and enhances the electron concentration and electrical conductivity. Consequently, the CrVN thin film electrodes achieve a remarkable specific capacitance of 22.8 mF cm-2 at 1.0 mA cm-2, along with excellent cycling performance (93.9% capacitance retention after 20,000 cycles at 5.0 mA cm-2). Furthermore, the assembled CrVN symmetric supercapacitor device exhibits a substantial energy density of 11.2 mWh cm-3 and an impressive power density of 7.5 W cm-3, respectively. These encouraging outcomes open new avenues for developing ternary TMNs-based electrodes for high performance supercapacitors.

Zinc-ion hybrid supercapacitors (ZIHCs) hold great promise in the realm of renewable energy storage. However, their development is severely hampered by the unsatisfactory practical capacity and poor stability. Herein, we report an effective strategy to improve the electrochemical performance by constructing hollow bimetallic nitride TiVN (H-TiVN) using a sacrificial template method. The optimized H-TiVN//Zn shows a high capacitance of 183.7 F g(-1) at 0.2 A g(-1) along with excellent stability (an 84.7% capacitance retention after 20,000 cycles at 5 A g(-1)). More importantly, the energy density can reach 57.42 Wh kg(-1), accompanied by a power density of 249.35 W kg(-1). Our work not only establishes H-TiVN as a high-performance electrode material for ZIHCs but also provides a general strategy for improving the electrochemical performance of nanomaterial electrodes.

Aqueous Zn batteries, which use metallic Zn as anodes, have gained significant attention due to their affordability and high safety standards. However, these Zn anodes are plagued by issues such as Zn dendritic growth and side reactions, including corrosion and hydrogen evolution. One straightforward yet effective approach to mitigate these issues is to apply protective coatings to the Zn anodes to enhance their reversibility. It is generally believed that these protective layers should have a high affinity for Zn. Contrarily, this study proposes that non-conductive coatings should form a strong binding with H+ ions while maintaining a weaker interaction with Zn2+ ions, thereby ensuring a higher selectivity for H+ over Zn2+. This concept is illustrated using zirconium dioxide (ZrO2), an ionic conductor that meets these criteria and effectively curbs side reactions and dendritic growth of Zn. Remarkably, Zn anodes coated with ZrO2 layer demonstrate a lifespan exceeding 6000 h at 1 mA cm(-2) and 1 mAh cm(-2), significantly outperforming uncoated ones, which last <200 h. This discovery introduces a novel design principle for insulating surface coatings, potentially applicable not only for Zn but also for other metal anodes.

Fe2O3 is one of the most common anode materials beyond carbons but suffers from unsatisfactory capacity and poor stability, which are associated with the insufficient utilization of active material and the structural instability caused by the phase transformation. In this work, we report an effective strategy to overcome the above issues through electronic structure optimization by constructing delicately designed Fe2O3@VN core-shell structure. The Fe2O3@VN/CC exhibits a much higher areal capacity of 254.8 mC cm-2 at 5 mA cm-2 (corresponding to 318.5 mF cm-2, or 265.4 F g-1) than the individual VN (48 mC cm-2, or 60 mF cm-2) or Fe2O3/CC (93.36 mC cm-2, or 116.7 mF cm-2), along with enhanced stability. Moreover, the assembled asymmetric supercapacitor devices based on Fe2O3@VN/CC anode and RuO2/CC cathode show a high stack energy density of 0.5 mWh cm-3 at a power density of 12.28 mW cm-3 along with good stability (80% capacitance retention after 14000 cycles at 10 mA cm-2). This work not only establishes the Fe2O3@VN as a high-performance anode material but also suggests a general strategy to enhance the electrochemical performance of traditional anodes that suffer from low capacity (capacitance) and poor stability.

: Aqueous zinc batteries are considered as a promising candidate for large-scale energy storage systems, alternative to lithium-ion batteries, due to the high safety and environmental friendliness. However, the cathode materials suffer from issues such as structural collapse and side reactions, which seriously restrict their commercialization. Since these issues are highly relevant to the surface and interface properties of cathode materials, the surface and interface engineering therefore is expected to improve the overall performance. This review first discusses the reaction mechanisms of various cathode materials, and then systematically summarizes and analyzes the recent progress of surface and interface engineering strategies, and finally provides a perspective on future directions, aiming to provide useful guidance for the design and preparation of cathode materials with high capacity and stability.

Electrocatalytic hydrogenation (ECH) of organics using water as hydrogen donors has been regarded as a green organic reduction technique to replace traditional chemical reactions that use sacrificial chemicals. The development of ECH process provides potential applications in the production of value-added chemicals owing to its low energy consumption, low pollution, high safety, and superior sustainability. However, its application is limited by the low conversion rate and poor selectivity toward desired products. The efficiency of ECH can be improved by rational design of electrocatalysts. This review covers several representative electrocatalytic systems (aldehydes, ketones, phenolic organics, alkynes, and organonitrogen compounds) and summarizes different ECH mechanisms, followed by thorough discussion on the modification strategies of electrocatalysts that are currently adopted to enhance the catalytic performance. Finally, in view of the current challenges for ECH, we discuss possible future directions in the field, aiming to provide guidance to the catalyst design toward highly efficient ECH reactions over different organic feedstocks.

The traditional technologies for industrial and agricultural effluent treatment are often energy-intensive. Herein, we suggest an electrochemical redox strategy for spontaneous and simultaneous decontamination of wastewater and generation of both fuels and electricity at low cost. Using hydrazine and nitrate effluents as a demonstration, we propose a hydrazine-nitrate flow battery (HNFB) that can efficiently purify the wastewater and meanwhile generate both ammonia fuel and electricity with the assistance of our developed bimetallic RuCo precatalyst. Specifically, the battery delivers a peak power density of 12 mW cm(-2) and continuously operates for 20 h with an ammonia yield rate of ca. 0.38 mmol h(-1) cm(-2) under 100 mA cm(-2). The generated electricity can further drive a hydrazine electrolyzer to produce hydrogen fuel. Our work provides an alternative pathway to purify wastewater and generate high value-added fuels at low cost.

Zinc (Zn) metal anodes suffer from the dendrite growth and hydrogen evolution reaction (HER) in classical aqueous electrolytes, which severely limit their lifespan. We propose a rational design of AgxZny protective coatings with selective binding to Zn2+ against H+ to simultaneously regulate the Zn growth pattern and the HER kinetics. We further demonstrate that by tuning the composition of the AgxZny coating the Zn deposition behavior can be readily tuned from the conventional plating/stripping (on Zn-AgZn3 coating) to alloying/dealloying (on Ag-AgZn coating), resulting in precise control of the Zn growth pattern. Moreover, the synergy of Ag and Zn further suppresses the competitive HER. As a result, the modified Zn anodes possess a significantly enhanced lifespan. This work provides a new strategy for enhancing the stability of Zn and potentially other metal anodes by precisely manipulating the binding strength of protons and metal charge carriers in aqueous batteries.

The acidic oxygen evolution reaction (OER) has long been the bottleneck of proton exchange membrane water electrolyzers given its harsh oxidative and corrosive environments. Herein, we suggest an effective strategy to greatly enhance both the acidic OER activity and stability of Co3O4 spinel by atomic Ru selective substitution on the octahedral Co sites. The resulting highly symmetrical octahedral Ru-O-Co collaborative coordination with strong electron coupling effect enables the direct dioxygen radical coupling OER pathway. Indeed, both experiments and theoretical calculations reveal a thermodynamically breakthrough heterogeneous diatomic oxygen mechanism. Additionally, the active Ru-O-Co units are well-maintained upon the acidic OER thanks to the electron transfer from surrounding electron-enriched tetrahedral Co atoms via bridging oxygen bonds that suppresses the overoxidation and thus dissolution of active Ru and Co species. Consequently, the prepared catalyst, even with a low Ru mass loading of ca. 42.8 μg cm-2, exhibits an attractive acidic OER performance with a low overpotential of 200 mV and a low potential decay rate of 0.45 mV h-1 at 10 mA cm-2. Our work suggests an effective strategy to significantly enhance both the acidic OER activity and stability of low-cost electrocatalysts.

The electrocatalytic nitrate reduction reaction (NtrRR) has recently become an emerging technology that can convert nitrate pollutants into high-value added ammonia products in a mild manner. However, it is highly challenging to develop NtrRR electrocatalysts with high activity, selectivity, and stability given the sluggish kinetics and diverse pathways of the NtrRR. Herein, we develop a Ru/beta-Co(OH)(2) heterostructure catalyst derived from in situ reconstruction of Ru-doped Co metal nanosheets with an ultralow Ru/Co ratio of 3.08 at%. The synergy and strong interactions between interfacial Ru and Co sites weaken the d-p orbital hybridization ability with *NH3 intermediates, which thus lowers the barrier of the potential determining step. As a result, the catalyst delivers an industrial-level current density of -500 mA cm(-2) at a positive potential of only 0.01 V vs. the reversible hydrogen electrode, along with a high ammonia Faradaic efficiency of 98.78%. Meanwhile, it can purify the nitrate sewage and reduce the nitrate concentration to 13-31 ppm. Furthermore, the assembled Zn-nitrate flow battery also delivers a decent power density of 29.87 mW cm(-2) and a high ammonia yield of up to 0.38 mmol h(-1) cm(-2) with excellent stability. This work suggests an effective strategy for designing high-performance electrocatalysts through interface engineering by rational reconstruction.

Electron-deficient Ru sites at Ru/Co(OH)2heterointerfaces weaken the d–p orbital hybridization ability and further facilitate the desorption of ammonia intermediates, thereby achieving ultrahigh nitrate electroreduction activity towards ammonia.

We propose an acid-alkaline furfural hybrid battery that can achieve a discharging power density of 47 mW cm-2 under 100 mA cm-2 energy output with a H2 faradaic efficiency (FE) up to ca. 200% and a furoate FE of around 97% with the aid of our developed Pt-Cu electrocatalyst.

Developing high-efficiency electrode materials is of great importance in manufacturing supercapacitor devices with superior electrochemical performance. Herein, we for the first time report a binder-free method for controllable growth of Cu3N electrode materials via magnetron sputtering for supercapacitor applications. Benefiting from their unique polyhedral structure and good electrical conductivity, Cu3N electrodes can achieve an areal capacity of 90.7 mC cm-2 at 1 mA cm-2 and outstanding cycling stability with a capacity retention of 97.4% after 20 000 cycles. In particular, the assembled Cu3N//active carbon quasi-solid-state asymmetric supercapacitor can exhibit a maximum energy density of 13.2 μW h cm-2 and a power density of 4.8 mW cm-2 with an operating voltage of 1.6 V. These remarkable performances demonstrate the great potential of sputtered Cu3N electrode materials for future energy storage applications.

The application of proton exchange membrane water electrolyzer (PEMWE) technology has long been limited by the excessive energy consumption and poor catalyst durability because of the harsh corrosive and oxidative conditions that are related to the anodic oxygen evolution reaction (OER) in acidic electrolytes. Herein, we circumvent this challenge by adopting alternative hydrazine oxidation reaction (HzOR) as the anodic half-reaction, integrated with the cathodic hydrogen evolution reaction (HER) for sustainable hydrogen production. To this end, we further developed a PtCo alloy nanosheets electrocatalyst that can efficiently catalyze both the HzOR and HER with ultralow potentials. Specifically, the overall hydrazine splitting driven by the PtCo alloy requires only 0.28 V at 10 mA cm(-2) along with outstanding stability of more than 3000 h. We further proposed a PEM hydrazine electrolyzer (PEMHE) design to promote the practical application. The device can not only produce hydrogen with a high yield rate of 1.87 mmol h(-1) cm(-2) at a practical current density of 100 mA cm(-2) with a long durability of 60 h, but also effectively decontaminate hydrazine sewage with the hydrazine removal efficiency up to 100%. Our work provides a new solution to simultaneous mass hydrogen fuel production and hydrazine hazard removal from acidic waste water at minimized energy consumption. (C) 2022 Published by Elsevier Ltd.