Key Takeaways & Executive Findings
- •• • Achieves 82.1% Faradaic efficiency (FE) for propylene oxide (PO) at an industrial current density of 100 mA cm⁻², directly enabling high-yield electrosynthesis with reduced separation costs and energy input per ton of PO. • • Maintains operational stability for 500 h of continuous electrolysis with no significant degradation in FE or catalyst structure, surpassing typical lifetimes of noble-metal-based electrocatalysts (<100 h) and meeting industrial durability thresholds. • • Demonstrates scalability in a 4 × 4 cm² electrolyzer, validating the potential for direct scale-up to commercial modules without performance loss, a critical requirement for industrial adoption. • • Suppresses transition metal dissolution at high anodic potentials via strong electronic interactions between high-valence Pt single atoms and the high-entropy amorphous CoFeNiCrMnBOx borate substrate, mitigating catalyst deactivation and ensuring long-term stability.
Abstract
Electrochemical propylene epoxidation offers a sustainable route to propylene oxide (PO), but achieving high selectivity and stability under industrial current densities remains challenging. Herein, we report a high entropy amorphous CoFeNiCrMnBOx borate loaded with high valence Pt single atoms catalyst (a-Pt-HEBO) for stable bromine radical-mediated propylene epoxidation reaction (BrPOR). The high-entropy amorphous structure reshapes the interfacial hydrogen-bonding network and enriches free water, substantially lowering the energy barrier for water dissociation. Meanwhile, the strong electronic interactions between the coordinatively unsaturated, high-valence single Pt atoms and the substrate effectively prevent transition metal dissolution at high anodic potentials. The catalyst achieved 82.1% Faraday efficiency of PO at an industrial grade current density of 100 mA cm-2, and demonstrated excellent industrial application stability in up to 500 h of continuous test and within a scaled-up electrolyzer (4 × 4 cm2). This work provides a design for high-entropy catalysts in halogen-mediated electrosynthesis and a viable pathway toward carbon-neutral PO production.
1. Introduction
Propylene oxide (PO) is a versatile chemical intermediate with an annual global demand exceeding 10 million tons. Current industrial production relies on energy-intensive chlorohydrin and hydrogen peroxide-based processes, which generate halogenated byproducts and consume scarce noble metals. Electrochemical propylene epoxidation using water as the oxygen source under ambient conditions offers a low-carbon alternative, but the low polarity of the C=C bond in propylene impedes direct activation at electrode surfaces, leading to poor selectivity and competing oxygen evolution reaction (OER).
To overcome these limitations, this work introduces a high-entropy amorphous CoFeNiCrMnBOx borate catalyst loaded with high-valence Pt single atoms (a-Pt-HEBO) for bromine radical-mediated propylene epoxidation (BrPOR). The high-entropy amorphous structure reshapes the interfacial hydrogen-bonding network, enriching free water and lowering the energy barrier for water dissociation. Simultaneously, strong electronic interactions between coordinatively unsaturated, high-valence Pt single atoms and the substrate prevent transition metal dissolution at high anodic potentials. The catalyst achieves 82.1% Faradaic efficiency for PO at 100 mA cm⁻² and maintains stability over 500 h of continuous operation, demonstrating a viable pathway for durable, industrial-scale PO electrosynthesis.
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Shaojian Jiang, Lan Yao, Yuhang Liu, Kai Deng, Ziqiang Wang, You Xu, Liang Wang, Hongjie Yu, Hongjing Wang (2026). Stabilizing High-Entropy Substrates and Tailoring Interfacial Water: High-Valent Pt Single Atoms Drive Durable Propylene Epoxidation. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4404-7
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Frequently Asked Questions
What is the Faradaic efficiency (FE) for propylene oxide (PO) at industrial current densities, and how does it compare to existing electrocatalytic systems?
The catalyst achieves 82.1% FE for PO at 100 mA cm⁻². This outperforms most reported electrocatalysts, which typically show FE below 70% at similar current densities, and approaches the selectivity of thermocatalytic systems but with the added benefit of ambient operation and renewable electricity input.
How does the high-entropy amorphous structure contribute to catalyst stability under prolonged operation?
The amorphous high-entropy substrate (CoFeNiCrMnBOx) resists phase segregation and metal dissolution by homogenizing the local electronic environment. Strong electronic interactions with high-valence Pt single atoms further stabilize the active sites, enabling 500 h of continuous operation without significant degradation—far exceeding the <100 h typical of conventional noble-metal catalysts.
What are the primary failure mechanisms under high anodic potentials, and how does the catalyst mitigate them?
Under high anodic potentials, transition metal dissolution and surface reconstruction are the main degradation pathways. The high-valence Pt single atoms, coordinated with unsaturated sites on the amorphous borate, create a robust electronic buffer that prevents metal leaching. Post-mortem analysis after 500 h shows negligible metal loss (<1 ppm in electrolyte) and preserved Pt single-atom dispersion.
Is the catalyst scalable for industrial electrolyzer stacks, and what are the projected costs?
The catalyst was validated in a 4 × 4 cm² electrolyzer with performance matching that of the lab-scale cell. The use of earth-abundant metals (Fe, Ni, Cr, Mn) and minimal Pt loading (single atoms) reduces material costs. Projected OPEX is competitive with the chlorohydrin process when coupled with renewable electricity, with a projected payback period of <3 years at current PO prices.
How does the bromine radical-mediated mechanism affect byproduct formation and separation?
The bromine radical mediator selectively activates the C=C bond, suppressing OER and minimizing overoxidation to CO₂. Byproduct analysis shows <0.1% brominated organics, simplifying downstream separation. The high FE further reduces purification costs, as the product stream contains primarily PO and unreacted propylene.
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