Molecular Coordination Engineering Enables Aminoethyl Phosphonic Acid as a Multifunctional Additive for High-Performance Zinc-Iodine Flow BatteriesShi, Han; Cui, Jing; Liu, Zhikun; Kang, Peng
doi: 10.1007/s12209-026-00488-ypmid: N/A
The practical application of aqueous zinc-ion batteries is critically hindered by the instability of the zinc metal anode, which suffers from uncontrollable dendrite growth and detrimental side reactions. Conventional electrolyte additives often focus solely on homogenizing the zinc-ion flux, while neglecting the pivotal role of crystallographic regulation. Herein, we propose a fundamental strategy to manipulate zinc deposition behavior through selective molecular adsorption. We introduce 2-aminoethylphosphonic acid (AEP) as a novel electrolyte additive that preferentially adsorbs onto the (100) and (101) crystal planes of zinc, as confirmed by experimental evidence from electric double-layer capacitance measurements, and theoretical DFT calculations, which reveal a lower adsorption energy on the (002) facet. Consequently, the AEP-modified electrolyte enables a densely packed zinc morphology and a significantly optimized interface, which collectively contribute to markedly enhanced electrode kinetics and cycling stability. The improved negative electrolyte enables the zinc-iodine flow battery (ZIFB) to operate for 600 h (1500 cycles) with a high energy efficiency (> 83%) at 80 mA/cm2. This work underscores the critical importance of crystallographic engineering via selective molecular adsorption. The mechanistic insights gained into the dual regulation of solvation structure and interfacial growth provide a new design principle for advanced electrolytes targeting highly reversible metal anodes.
Revealing Electron Transfer Dynamics in a ZnIn2S4/PDA S-scheme Photocatalyst via Fs-TASHu, Chenrui; Yang, Songyu; He, Bowen; Cheng, Bei ; Tan, Haiyan; Zhang, Jianjun; Yu, Jiaguo
doi: 10.1007/s12209-026-00487-zpmid: N/A
Single-component ZnIn2S4 (ZIS) exhibits rapid charge recombination, resulting in low photocatalytic efficiency. To address this issue, the construction of an S-scheme heterojunction is a feasible strategy. Herein, a ZIS/dopamine (PDA) S-scheme heterojunction photocatalyst was successfully fabricated by depositing PDA onto the surface of ZIS nanoflowers. The optimized ZIS/PDA composite shows a significantly improved H2 production rate compared to pure ZIS and PDA. In situ irradiated X-ray photoelectron spectroscopy provides steady-state spectral evidence of S-scheme electron transfer from ZIS to PDA upon photoexcitation. Furthermore, transient spectral evidence for the ZIS/PDA S-scheme heterojunction is revealed via femtosecond transient absorption spectroscopy. Analysis of the charge dynamics in the ZIS component identifies an additional ultrafast lifetime component in the ZIS/PDA composites. This newly identified component is primarily attributable to the S-scheme interfacial electron transfer channel. The S-scheme electron transfer process gradually accelerates with increasing PDA concentration, ultimately reaching an optimal interfacial electron transfer lifetime of 0.9 ps. This ultrafast electron transfer dynamics facilitates the participation of photogenerated charge carriers in photocatalytic H2 evolution. Overall, this study provides new insights into the transient spectral analysis of S-scheme photocatalysts.
Theoretical Study on the Regulation of CO Preferential Oxidation Performance of Pt1@FeOx Single-Atom Catalysts by Selective Orbital CouplingZheng, Xiuhui; Li, Yaqian; Cao, Jianlin; Wei, Sheng; Yin, Defu; Yan, Hao; Tuo, Yongxiao; Feng, Xiang; Yang, Chaohe; Chen, De
doi: 10.1007/s12209-026-00489-xpmid: N/A
Preferential oxidation of CO (CO-PROX) is essential for H2 purification in proton-exchange membrane fuel cells. Understanding the intrinsic electronic structural factors that influence catalytic performance is key to rational catalyst design. Using Pt single-atom catalysts supported on Fe2O3 and Fe3O4 as model systems, this work systematically investigates the relationship between structure and performance, focusing on the strength of selective orbital coupling and CO-PROX activity. On both supports, Pt single atoms are stabilized in an embedded form by substituting lattice Fe sites (Pt1@FeOx). Furthermore, CO and H2 are preferentially activated at Pt-lattice O bridge sites, while O2 activation occurs at Pt sites. Compared to the Pt1@Fe3O4 system, the Pt1@Fe2O3 system exhibits higher theoretical activity and selectivity, with energy barriers of 0.28 eV for CO oxidation and 0.87 eV for H2 oxidation. The enhanced performance of Pt1@Fe2O3 stems from its higher lattice O redox activity and an optimal selective orbital coupling strength, measured by the descriptor Σ|Δε| (the absolute value sum of band‑center shifts for the dominant interacting orbitals). This creates a clear energetic preference for activating CO over H2. This study establishes a semiquantitative structure–activity relationship linking electronic structure, adsorption strength, and catalytic performance, providing concrete theoretical guidance for experimental design of high-performance CO-PROX catalysts.
Electrocatalytic Valorization of Biomass: Selective C–X Bond Cleavage and ConstructionZhang, Xue; Chen, Lang; Zhang, Zixuan; Wang, Hua; Zhang, Shengbo
doi: 10.1007/s12209-026-00490-4pmid: N/A
Biomass valorization represents a critical frontier in green chemistry and energy chemistry, where the essence of transformation lies in the selective cleavage and reconstruction of key chemical bonds. Electrocatalysis, characterized by mild operating conditions and an environmentally benign nature, offers a highly promising and sustainable pathway for upgrading waste biomass into value-added products. From the perspective of chemical bonds, this review systematically summarizes the latest research progress in electrocatalytic biomass valorization. First, the underlying microscopic electron/proton transfer mechanisms involved in electrocatalytic oxidation and reduction are discussed. Next, the cleavage and reconstruction of key chemical bonds, including C–H, C–O, C–C, C–N, and C–S bonds, are highlighted, with an in-depth analysis of substrate activation mechanisms, reaction pathways, and corresponding catalyst design strategies. Additionally, this review analyzes the regulatory mechanisms by which the interfacial microenvironment governs the conversion selectivity of different chemical bonds. Finally, perspectives on the core challenges currently facing this field are provided, including the insufficient elucidation of dynamic reaction mechanisms, the limited development of industrial-grade and stable catalysts, and the slow progress in scaling up electrolysis devices and processes. This review aims to provide theoretical guidance and new insights for the rational design of highly selective electrocatalysts for biomass valorization.Graphical AbstractThis review summarizes key advances in electrocatalytic biomass valorization from the perspective of chemical bonds, focusing on the selective cleavage and reconstruction of C–H, C–O, C–C, C–N, and C–S bonds, substrate activation pathways, and rational catalyst design, offering theoretical guidance for designing highly selective electrocatalysts for biomass upgrading.[graphic not available: see fulltext]