EES catalysis最新文献

In this work, we demonstrate the inversion of the classical bottom-up approach to drive the discovery of improved energy conversion electrocatalysts top-down. Starting with complex alloy catalysts of many constituents, we down-select to optimal materials by removing low-performing elements from the alloy. The efficiency of this data-driven approach arises from the fact that when studying many elements together in one material, information is also obtained on the less complex alloys that contain fewer constituents. Therefore, the number of experiments required to study the complex alloy is fewer than those needed for studying all constituent alloys individually. In addition, this top-down approach allows for a new way of comparing activity models constructed from experimental data with theoretical simulations. We introduce the approach by studying the Au-Ir-Os-Pd-Pt-Re-Rh-Ru high entropy alloy (HEA) composition space for the acidic oxygen reduction reaction (ORR). By studying 200 compositions, we created a machine-learned activity model and provide evidence that the model can predict the activity of underlying, less complex compositions that are contained in the Au-Ir-Os-Pd-Pt-Re-Rh-Ru HEA composition space.

As we welcome the first issue of EES Catalysis in 2026, it is inspiring to reflect on how far our community has progressed in such a short period. Since its launch in 2023, EES Catalysis has rapidly evolved from a new open-access journal into a vibrant platform that unites scientists working across all aspects of energy and environmental catalysis. Building on the strong momentum of 2024 and 2025, the journal continues to champion impactful, interdisciplinary research that addresses some of the most urgent challenges faced by our planet.

Electrochemical CO₂ reduction (ECR) to formate/formic acid (FA) represents one of the most viable pathways for converting CO₂ into value-added chemicals, particularly under industrially relevant conditions. However, long-term operational stability of gas diffusion electrodes (GDEs) at high current densities remains a critical bottleneck. Herein, we report the development of carbon-free bismuth (Bi) and tin (Sn)-based GDEs fabricated via a custom methodology that enables stable ECR operation for over 4000 hours (Bi) and 1050 hours (Sn) at 100 mA cm⁻², achieving faradaic efficiencies (FE) of up to 90% and 70%, respectively. A comprehensive mechanistic investigation reveals that performance degradation is predominantly driven by dynamic changes in the bulk catholyte, particularly pH shifts and HCO₃⁻ ionic depletion, rather than intrinsic catalyst decay. Control experiments and in situ Raman spectroscopy highlight the formation and regeneration of bismuth subcarbonate species as key intermediates in the ECR process. The results demonstrate sustained operation with periodic reactivation, rather than static stability, highlighting how electrolyte management and pulsed electrolysis can extend system durability under industrially relevant conditions. Crucially, we demonstrate that a combination of catholyte refreshment and periodic anodic pulsing reactivates electrode performance, sustaining high selectivity and suppressing the hydrogen evolution reaction (HER) over extended durations.

The development of efficient and stable oxygen evolution reaction (OER) electrocatalysts for seawater electrolysis is vital to enable sustainable hydrogen production in coastal and arid regions without further burdening scarce freshwater resources. Here, we report the design of an iron-modified cobalt–chromium layered double hydroxide (Fe–CoCr LDH) derived from a cobalt-based metal–organic framework (Co MOF) for the OER in alkaline seawater media. The synthesis was carried out entirely at room temperature using a rapid, solution-based process. The resulting Fe–CoCr LDH catalyst demonstrates high OER activity, achieving low overpotentials of 250, 300, and 320 mV at current densities of 100, 500, and 1000 mA cm⁻², respectively. Furthermore, the catalyst exhibits very good long-term stability in both 1 M KOH and 6 M KOH natural seawater, maintaining performance over 100 hours at 100 and 500 mA cm⁻². These results highlight the potential of earth-abundant transition metal-based LDHs as efficient OER electrocatalysts for seawater electrolysis applications.

Proton exchange membrane water electrolyzers (PEMWEs) are among the emerging technologies for hydrogen production due to their high operational current density, low operating temperature, and ultra-pure hydrogen production. However, industrial scale hydrogen production via PEMWEs is greatly hindered by the interrelated trio-factor of low performance, limited durability, and high cost. The iridium-based catalyst layer (CL) and platinum-coated titanium-based porous transport layer (PTL) are the core components which primarily contribute to the performance, durability and cost of PEMWEs. The degradation of costly CL and PTL (due to Ir and Pt usage) is a significant challenge for wider development of PEMWEs. In this review, we discuss the degradation of CL and PTL and provide an overview of the diagnostic techniques used to investigate the degradation processes. In situ and ex situ analysis reveal that the future development of CL should be focused on ink properties optimization and catalyst coated membrane fabrication methods, which affect the CL architecture and performance. Similarly, the titanium passivation, corrosion and increased interfacial contact resistance are the key factors that affect the PTL microstructure and performance. Thus, it is crucial to develop corrosion resistant coating and incorporation of low-cost materials as interlayers to reduce the cost without compromising the stability of PTL. The understanding of CL and PTL degradation and their characterization methods along with future perspectives will guide the development of durable and low-cost CL and PTL for wider applications of PEMWEs.

Three different electrocatalysts have been prepared, characterized, and applied to a high-temperature direct ethanol polymer electrolyte membrane electroreformer (DEPEME) based on the removal of surface Cu from the initial Pt_xCu/C (x = 3, 1, and 1/3) raw materials. The resulting structure consisted of a Pt-enriched shell on a PtCu alloy core deposited on C [alloyed Pt_xCu@Pt_yCu/C (y ≫ x)], achieved after the acid treatment of the prepared catalysts, in a core–shell (CS) configuration. This structure is confirmed by X-ray diffraction, which evidences the formation of a PtCu alloy, whereas X-ray photoelectron spectroscopy reveals an enriched Pt shell. Finally, transmission electron microscopy images revealed the dispersed deposition of metal nanoparticles at the nanoscale range. Regarding the electrochemical performance, the CS materials displayed enhanced CO tolerance and ethanol electro-oxidation (EEO) performance, characterized by increased current density and a lower onset potential compared to Pt/C. These results were corroborated at the high-temperature DEPEME condition of 150 °C. Moreover, the monitoring of the EEO products revealed that the CS PtCu materials notably enhanced the selectivity for CO₂, resulting in a desirable combination of high hydrogen production rate (0.205 kg of H₂ m⁻² h⁻¹) and CO₂ selectivity (close to 50%) at a reduced energy consumption (25.46 kWh kg H₂⁻¹). Finally, a techno-economic analysis presents the potential of using ethanol produced in a sugarcane plant from bagasse (second-generation) and estimates the cost of H₂ produced compared to that of a PEM water electrolyzer.

This work reports the highest photoelectrochemical (PEC) performance for selenium (Se)-based photocathodes, achieved through a simple, sustainable, and nanoparticle-free design. A half-cell solar-to-hydrogen (HC-STH) efficiency of 2.78 ± 0.01% and a photocurrent density of 11.35 ± 0.01 mA cm⁻² at 0 V_RHE were obtained with bare Mo/Se devices tested in H₂SO₄, surpassing the previous Se-based (FTO/Se/TiO₂/Pt) HC-STH benchmark by over a factor of seven. To improve sustainability and device safety, the deposition of a thin TiO₂ passivation layer enabled comparable performance (2.76 ± 0.01%), even in neutral phosphate buffer, allowing to obtain the highest photoelectrocatalytic onset potential reported so far (0.74 V_RHE). Unlike most PEC devices that rely on complex multilayer stacks and costly noble metals, which limit scalability and environmental compatibility, this work demonstrates that high performance can be achieved with a fully earth-abundant and low-toxicity materials set. A systematic screening of back contacts, Se phases, absorber thickness, protective overlayers, and electrolyte formulations revealed the crucial role of Mo in enhancing Se orientation, charge extraction, and photovoltage generation. These results establish multiple benchmarks for Se-based PEC water splitting and highlight the potential of streamlined and scalable architectures for efficient and sustainable green hydrogen production.

Thin-film-based catalysts, fabricated through physical vapor deposition, have attracted significant interest as promising materials for electrochemical CO₂ reduction. In this context, metallic Cu films function as active catalyst layers for the reduction to ethylene and ethanol. However, these films still experience high overpotentials, resulting in low energy efficiencies. In this study, we have fabricated Cu_1−xN_x films to overcome this issue by incorporating nitrogen into the sputtering process, leading to the formation of an anti-ReO₃ crystal structure of Cu₃N, which contains interstitial vacancies filled with Cu atoms. Under optimal sputtering conditions of r_N2 = 0.50, sputter rate = 4 Å s⁻¹, and pressure = 6 μbar, EDX analysis reveals a sub-stoichiometric thin-film composed of Cu_0.84N_0.16. In the electrochemical CO₂ reduction, this film resulted in an increase in energy efficiency from 15.8% to 20% for ethylene compared to pure Cu films, which was attributed to a decrease in the measured potential by ± 500 mV, due to the addition of nitrogen in the structure. This key finding suggests that for future applications, Cu_1−xN_x layers should be employed instead of metallic Cu to reduce the required energy demands while maintaining selectivity.

This work presents a one-dimensional continuum modeling approach to investigate various cell architectures used for electrochemical conversion of CO₂ to formate/formic acid. Ion transport is simulated by a system of generalized modified Poisson–Nernst–Planck (GMPNP) equations that reflect the reactive transport phenomena including steric effects as the electrolyte solutions become concentrated. In the cathode catalyst layer, ionic current contributions from both the supporting electrolyte and solid-state ionomer are considered. Voltage and CO₂ utilization breakdowns are utilized to deconvolute the impacts of the cell architecture. The origins of (bi)carbonate formation in the cathode are explored, as the subsequent decrease in CO₂ availability is a key reason for low faradaic efficiencies to formate/formic acid. In addition, the role of a supporting electrolyte (KOH) is investigated to understand its tradeoffs: while the K⁺ ions can improve both conductivity and electrochemically active surface area in the cathode, the presence of OH⁻ ions raises the pH and leads to deleterious formation of (bi)carbonates. To this end, we also present parametric studies on the concentration and flow rate of supplied KOH to the cell, to establish a path towards eliminating the need for a supporting electrolyte.

Platinum-group metal-free single-atom catalysts (SACs) are vital for cost-effective fuel cells, yet their adoption is hindered by performance limitations and challenges in scalable production. While Fe–N–C SACs offer high activity, their stability is severely compromised by Fenton-induced degradation. To address this, Co–N–C SACs have emerged as promising alternatives due to their much lower Fenton activity and hence improved durability. However, conventional synthesis relies on solvent-intensive methods, limiting large-scale, environmentally friendly production and precise structural control. Here, we report a solid-phase synthesis strategy via the Kirkendall effect for the kilogram-scale production of Co-doped zeolitic imidazolate framework-8 (Co-ZIF-8) with high reproducibility and precise compositional control. Further pyrolysis at high temperatures enables the formation of structurally well-defined Co–N–C SACs with tunable composition, high site density, and superior scalability. The optimized catalyst, when integrated as the cathode in a representative proton exchange membrane fuel cell (PEMFC) system, delivers remarkable power densities of 0.70 W cm⁻² and 0.39 W cm⁻² in O₂ and air conditions, respectively, outperforming most reported Co-based catalysts. This work establishes a generalizable and environmentally sustainable route for the large-scale production of high-performance non-precious metal electrocatalysts, advancing PEMFC technology and broader electrochemical energy applications.