Haozhe Zhang

Electrochemical carbon dioxide reduction reaction (eCO ₂ RR) provides a pathway to convert CO ₂ into value‐added chemicals. Here, we report a family of carbon‐supported tin–copper (Sn–Cu) bimetallic catalysts synthesized via an amalgamated lithium metal (ALM) method with controlled tuning of metal dispersion from isolated atoms to nanocrystallites. As metal loadings increase, the catalyst structure evolves from atomically dispersed Sn‐Cu dual sites (Sn _1.5 Cu/C‐0.75) to Sn‐rich nanodomains (Sn ₃ Cu/C‐13) and Cu/Sn crystallites (Sn ₃ Cu/C‐24), leading to a systematic shift in CO ₂ RR selectivity from acetaldehyde to formate at low overpotentials. Notably, Sn _1.5 Cu/C‐0.75 achieves a Faradaic efficiency of 49.7% for acetaldehyde at −0.5 V versus the reversible hydrogen electrode. The CO ₂ conversion pathways behind these selective, size‐modulated catalysts are elucidated by structural characterization, together with electrochemical analysis of structure‐selectivity correlations, establishing a clear structure‐property relationship for tuning CO ₂ RR pathways.

Aqueous Zn-organic batteries are promising due to the sustainability and tunability of organic cathodes. However, the critical challenge in their practical application lies in dissolution, degradation, and sluggish kinetics, ultimately degrading the cycling stability and rate capability. Herein, we demonstrate a simple effective electrolyte engineering strategy by introducing potassium chloride (KCl) as a co-solute into the ZnCl ₂ electrolyte to achieve high-performance Zn batteries utilizing 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) as the cathode. Experimental studies and molecular dynamics simulations reveal that KCl addition not only enhances electrolyte conductivity but also modulates Zn ²⁺ solvation environment to form [Zn(H ₂ O) ₂ Cl ₄ ] ²⁻ , significantly improving ion diffusion kinetics. Consequently, the Zn//PTCDA in the ZnCl ₂ -KCl electrolyte exhibits a remarkable capacity of 124.7 mAh g ⁻¹ with an average voltage of 0.65 V, exceptional rate performance (56% capacity retention at 30 A g ⁻¹ ), and prolonged cycling performance (90.9% retention after 10,000 cycles). Experimental and density functional theory mechanistic studies unveil a new reversible Zn ²⁺ /K ⁺ co-storage mechanism in the PTCDA cathode, where K ⁺ acts as a charge shield and structural pillar, synergistically decreasing the ion migration energy barrier, enhancing reaction kinetics, and stabilizing the cathode structure. This work elucidates dual-ion storage chemistry and highlights rational electrolyte design for durable, high-power metal–organic batteries.

We report an electrochemical CO₂ reduction reaction catalyzed by a paramagnetic and conductive CuO/Cu interface with spins polarized by a moderate external magnetic field (MF) of ∼800 gauss, achieving a ∼30% increase in CO₂-to-C₂₊ Faradaic efficiency (FE) compared to that in the absence of the MF in a flow cell electrolyzer. At a current density of 400 mA/cm², the CO₂-to-C₂₊ FE reached 86.7 ± 2.7% with 47.9 ± 1.4% cathodic energy efficiency (EE) in contrast to the CO₂-to-C₂₊ FE of 67.6% with 36.4% of EE in the absence of MF. Notably, ethanol production exhibits a much higher response to the MF (∼55.6% increase in FE) than ethylene (∼6.4% increase in FE) at 400 mA/cm². In situ surface-enhanced Raman spectroscopy (SERS) captured magnetic-field-enhanced *CO coverage and ethanol-forming C₂ intermediates on CuO/Cu, providing direct spectroscopic evidence of spin-modulated pathway selection. Computational study suggests that the enhancement of ethanol selectivity is due to the reduced reaction kinetic barrier under MF, while the ethylene selectivity is less affected, mainly due to the insensitivity of the kinetic barriers under MF.

In the face of growing global energy demands, the development of efficient and safe energy storage technologies is of critical importance. Aqueous zinc-based batteries (AZBs) demonstrate promising potential for large-scale energy storage due to their inherent safety, abundant zinc reserves, low cost, and relatively high energy density. However, the widespread application of AZBs is hindered by several challenges, including dendrite growth and side reactions on the zinc anode, as well as dissolution and structural degradation of cathode materials. Metal-organic frameworks (MOFs), characterized by their well-defined and controllable crystal structures, tunable pore environments, and highly designable chemical compositions, present a versatile solution for tackling these challenges. This review systematically summarizes recent progress in the application of MOFs and their derivatives in AZBs, focusing on design strategies and underlying mechanisms for performance optimization when they are employed as high-performance electrode materials, multifunctional interfacial protective layers, separator modifiers, and solid-state electrolytes. Finally, this review discusses the existing challenges and controversies in current research and offers forward-looking perspectives and suggestions for the future development of MOF-based advanced AZBs.

Large-scale battery manufacturing requires understanding the fundamental principles of materials and interfaces and relies on advanced techniques for detailed interrogation. Despite advancements in the industrial scale production and their associated quality control tools, challenges such as electrode heterogeneity, internal defects, and large-scale material waste (e.g. scrap) can hamper manufacturing. Synchrotron X-ray characterization techniques offer spatial, temporal, chemical resolution that can provide diagnostic insights into for metrology across various manufacturing steps. This review examines the use of synchrotron tools to advance understanding of key steps in the battery manufacturing process. Recent examples demonstrate how synchrotron methods resolve manufacturing challenges and uncover degradation pathways that are otherwise inaccessible. Future directions for advancing battery manufacturing emphasize collaboration between academia and industry through the use of synchrotron X-ray techniques.

Designing organic fluorescent molecules with tailored optical properties has been a long-standing challenge. Recently, statistical models have opened new avenues for tackling this problem. Inverse design has attracted considerable attention in organic materials science; however, most existing approaches focus on arbitrary design or theoretical properties. Here, we introduce a strategy that enables the direct optimization of specific experimental properties during the inverse design process. Our method employs an adaptive β-variational autoencoder (adaptive β-VAE) combined with a latent vector-based prediction model. By dynamically tuning the Kullback–Leibler divergence scaling factor (β) and employing a separate training strategy, we enhance both the robustness of the generator and the diversity of the generated molecules. We demonstrate that latent vectors from the adaptive β-VAE serve as powerful inputs for downstream prediction models of experimental properties, such as fluorescence energy and quantum yield. Our optimized search framework for organic fluorescent materialsguided by gradients in latent space and validated by newly synthesized molecules sampled from optimal regions in the high-dimensional spaceshows strong potential for broader applications in the design of diverse organic materials.

Electrodepositing metal materials in large capacity, at low potential, and with high reversibility serves as the foundation for any aqueous rechargeable battery chemistry to realize the promises of high energy, low cost, and high safety. However, such a foundation is not solid because of the natural tendency of metals to form irregular, nonplanar, and often dendritic morphologies during electrochemical crystallization, which is further amplified in an acidic environment due to the faster kinetics of the coupled proton and mass-transport processes between hydrated metal ions and free metal atoms. As a typical representative, tin metal (Sn⁰) has potential to achieve high energy in acidic batteries, but its nonuniform large-particle morphology, obtained from traditional electrodeposition, leads to dead Sn⁰ formation and deteriorating reversibility, accompanied by the sustained hydrogen evolution reaction (HER) and active Sn⁰ loss. Here, we report quaternary onium salts as effective interfacial cocations that, via selective adsorption, steadily texturize Sn⁰ deposition along the (211) plane, which is intrinsically inert to the HER, thus regulating the film deposition process by favoring the formation of planar Sn⁰ film. Such Sn⁰ film brings exceptional reversibility in acidic electrolytes, which translates into sustained cycling stability at applicable areal capacities in both anode-half cells (∼1500 deposition/dissolution cycles at 5 mAh cm^-2) and full cells (350 charge/discharge cycles at 5 mAh cm^-2). Textured electrodeposition with intrinsic HER-suppression capability provides a universal solution for diverse metal anode materials in rechargeable energy-dense aqueous batteries.

Rechargeable aqueous batteries based on metallic anodes hold tremendous potential of high energy density enabled by the combination of relatively low working potential and large capacity while retaining the intrinsic safety nature and economical value of aqueous systems; However, the realization of these promised advantages relies on the identification of an ideal metal anode chemistry with all these merits. In this review, the emerging Sn metal anode chemistry is examined as such an anode candidate in both acidic and alkaline media, where the inertness of Sn toward hydrogen evolution, flat low voltage profile, and low polarization make it a unique metal anode for aqueous batteries. From a panoramic viewpoint, the key challenges and detrimental issues of Sn metal batteries are discussed, including dead Sn formation, self‐discharge, and electrolyte degradation, as well as strategies for mitigating these issues by constructing robust Sn anodes. New design approaches for more durable and reliable Sn metal batteries are also discussed, with the aim of fully realizing the potential of Sn anode chemistry.

Single-crystal layered oxides (SC-NMC) with grain boundary-free configuration, have effectively addressed the long-standing cracking issue of conventional polycrystalline Ni-rich cathodes (PC-NMC) for lithium-ion batteries, prompting a shift in optimization strategies. However, continued reliance on anisotropic lattice volume change—a well-established failure indicator in PC-NMC—as a metric for understanding lattice strain and guiding compositional designs for SC-NMC becomes contentious. Herein, leveraging multi-scale diagnostic techniques, we unraveled the distinct nanoscopic strain evolution in SC-NMC cathodes, challenging the conventional composition-driven strategies and mechanical degradation indicators used for PC-NMC. Through particle-level chemo-mechanical analysis , we reveal a decoupling between mechanical strain and lattice volume change of SC-NMC, identifying that the structural instability in SC-NMC is primarily driven by multiple-dimension lattice distortions induced by kinetics-driven reaction heterogeneity and progressively deactivating chemical phases. Consequently, the roles of cobalt (Co) and manganese (Mn) in SC-NMC have been redefined based on the newly established mechanical failure mode. Unlike cobalt’s detrimental role in PC-NMC, we find Co to be critical in enhancing the longevity of SC-NMC cathodes by mitigating localized lattice strain along extended diffusion pathway, whereas Mn exacerbates mechanical degradation. Our findings fundamentally redefine the compositional requirements for SC cathodes compared to conventional NMC cathode systems, offering new insights into developing mechanically robust electrode materials with high capacity and superior durability.

Safe and cost-effective aqueous acidic batteries (AABs) offer substantial promise for renewable energy storage, as it have the potential to achieve greater energy and power density by utilizing non-metal hydrate protons as charge carriers.¹ However, most of traditional aqueous anode electrodes (Zn, Fe, etc.) have incompatibility with AABs due to the instability in acid, resulting in the quite limited choice of anode materials in acidic environment. In prior research, we successfully demonstrated that Sn metal can serve as a highly suitable anode material for AABs.² This is attributed to its comparatively high overpotential for the hydrogen evolution reaction (HER), substantial theoretical capacity (451.6 mAh g⁻¹), and negative redox potential (−0.14 V vs. SHE).³ The critical issue is that Sn tends to form polyhedral particles during the electro-deposition due to the small difference in surface energy between different planes.⁴ Along with the increase of capacity, the polyhedron Sn particles may become detach and fragment, ultimately leading to the formation of inactive, or dead Sn, which significantly impacts the cycling stability of Sn anode and even cause severe HER. We will present our efforts of developing reversible Sn anode for AABs by regulating Sn metal growth. Our first work applies interfacial alloying regulation to achieve smaller grain size and more uniform Sn deposition by higher propensity for nucleation and Sn migration energy barrier, thus increased the anode reversibility. The following work successfully selected a HER-inert crystal plane and achieved its preferential growth used cationic surfactants electrolyte additive. A dense and compact Sn film is obtained by adjusting the adsorbed species on the Sn surface, and no dead Sn was observed after cycling. Based on these regulated Sn metal anodes, we demonstrated several Sn-based AABs (MnO₂//Sn, PbO₂//Sn, etc.), with promising performance on output voltages, specific energy densities, kinetics, and lifespans. References X. Wu, J. J. Hong, W. Shin, L. Ma, T. Liu, X. Bi, Y. Yuan, Y. Qi, T. W. Surta, W. Huang, J. Neuefeind, T. Wu, P. A. Greaney, J. Lu, X. Ji. Nat. Energy 2019, 4, 123-130. H. Zhang, D. Xu, F. Yang, J. Xie, Q. Liu, D. Liu, M. Zhang, X. Lu, Y. S. Meng. Joule 2023, 7, 971-985. W. Zhou, S. Ding, D. Zhao, D. Chao. Joule 2023, 7, 1099-1110. Y. Yao, Z. Wang, Z. Li, and Y. Lu. Adv. Mater. 2021, 33, 2008095.