Key Takeaways & Executive Findings
- •• Janus dual-atom catalyst (JDAC) with bifunctional centers was synthesized via a single-step bipolar doping strategy to promote efficient charge separation and superior electrocatalytic performance. • The in situ X-ray absorption near-edge structure and Raman spectroscopy analyses demonstrated that Ni and Fe centers in JDAC function as effective sites for oxygen evolution reaction and oxygen reduction reaction, and effectively suppress photoelectron recombination while enhancing photocurrent generation. • The assembled JDAC-based light-assisted rechargeable zinc–air batteries exhibited extraordinary stability at large current densities (300 cycles at 50 mA cm−2, and 6000 cycles at 10 mA cm−2 under light illumination). • This work provides pivotal insight into designing Janus dual-atom catalysts that efficiently convert solar energy into electric and chemical energy, advancing sustainable energy storage.
Abstract
Harnessing solar energy to enhance the rechargeable zinc–air batteries (RZABs) performance is a promising avenue toward sustainable energy storage and conversion. Simultaneously enhancing light-absorption capacity and carrier separation efficiency in nanomaterials, as well as improving electrical conductivity and configuration for electrocatalysis, presents a formidable challenge due to inherent trade-offs and interdependencies. Here, we have developed a Janus dual-atom catalyst (JDAC) with bifunctional centers for efficient charge separation and electrocatalytic performance through a bipolar doping strategy. The in situ X-ray absorption near-edge structure and Raman spectroscopy analyses demonstrated that the Ni and Fe centers in JDAC not only function as effective sites for oxygen evolution reaction and oxygen reduction reaction, respectively, but also serve as efficient hole and electron enrichment sites, effectively suppressing photoelectron recombination while enhancing photocurrent generation. As a result, the assembled JDAC-based light-assisted RZABs exhibited extraordinary stability at large current densities. This work delivers pivotal insight to design Janus dual-atom catalysts that efficiently convert solar energy into electric and chemical energy.
1. Introduction
Rechargeable zinc–air batteries (RZABs) have gained much interest as a promising energy storage technology due to their remarkable theoretical energy density (1086 Wh kg−1), cost-competitiveness, environmental friendliness, and high safety [1, 2]. In recent years, solar-driven ZABs harness photogenerated holes and electrons to facilitate redox reactions, offering an attractive strategy for solar-driven energy storage and conversion. By harnessing the power of light, the abundant solar energy provides additional acceleration for catalytic reactions in solar-driven batteries [3]. It is essential for a photocathode that possesses both photoresponsivity and efficient catalytic activity for oxygen redox reactions in light-assisted RZABs.
Current research on photocathode primarily concentrates on semiconductors such as BiVO4 [4], α-Fe2O3 [5], TiO2 [6, 7, 8], ZnO [9], poly(1,4-di(2-thienyl))benzene (PDTB) [10], polytrithiophene (pTTh) [11], and C3N4 [12]. However, these photocathodes exhibit a wide bandgap (2.3 eV for BiVO4, 2.2 eV for α-Fe2O3, 3.1 eV for TiO2, and 2.7 eV for g-C3N4), which constrains their ability to absorb visible light. C4N, a novel semiconductor with a narrow bandgap of 1.99 eV, induces a favorable photocoupling effect with visible-light response for enhanced oxygen catalysis reactions [13, 14]. However, another important aspect is that current photoelectrocatalysts commonly suffer from a high recombination rate of photogenerated electron–hole pairs, which is pronounced at high current densities. As a consequence, the assembled light-assisted RZABs are limited to operate at low current densities (0.1 or 1 mA cm−2). In addition, photoelectrocatalysts encounter challenges such as limited conductivity and insufficient inherent electrocatalytic activity [15]. To address these limitations, recent researches explored several strategies, such as constructing heterojunctions [16, 17], introducing chemical dopants [18], tailoring defects [19, 20], and utilizing piezoelectric fields [21, 22]. Evidently, the optimization of light-absorption capacity and carrier separation efficiency for photocatalysis, as well as enhancement of electrical conductivity, remains a formidable challenge.
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Ning Liu, Yinwu Li, Wencai Liu, Zhanhao Liang, Bin Liao, Fang Yang, Ming Zhao, Bo Yan, Xuchun Gui, Hong Bin Yang, Dingshan Yu, Zhiping Zeng, Guowei Yang (2025). Engineering Bipolar Doping in a Janus Dual-Atom Catalyst for Photo-Enhanced Rechargeable Zn-Air Battery. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01707-2
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Frequently Asked Questions
What is a Janus dual-atom catalyst (JDAC) and how is it synthesized?
A Janus dual-atom catalyst (JDAC) is a catalyst with two different metal atoms (Ni and Fe) positioned asymmetrically, creating a Janus structure. It is synthesized via a single-step bipolar doping strategy, which introduces both electron-rich and electron-poor regions to enhance charge separation and electrocatalytic activity.
How does the bipolar doping strategy improve the performance of the catalyst?
Bipolar doping creates a built-in electric field that promotes efficient separation of photogenerated electron-hole pairs, suppresses recombination, and enhances photocurrent generation. It also provides bifunctional active sites (Ni for OER and Fe for ORR), improving overall electrocatalytic performance.
What are the key findings of the in situ X-ray absorption near-edge structure (XANES) and Raman spectroscopy analyses?
The analyses revealed that Ni and Fe centers in JDAC act as effective sites for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), respectively. They also serve as hole and electron enrichment sites, effectively suppressing photoelectron recombination and enhancing photocurrent generation.
What stability does the JDAC-based light-assisted rechargeable zinc-air battery exhibit?
The assembled battery demonstrated extraordinary stability at large current densities, achieving 300 cycles at 50 mA cm−2 and 6000 cycles at 10 mA cm−2 under light illumination, indicating excellent durability for practical applications.
What is the significance of this work for sustainable energy storage?
This work provides pivotal insight into designing Janus dual-atom catalysts that efficiently convert solar energy into electric and chemical energy, offering a promising strategy to enhance the performance of photo-enhanced rechargeable zinc-air batteries and advance sustainable energy storage technologies.
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