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Cu is a unique metal that catalyzes carbon monoxide/carbon dioxide (CO/CO2) to form high-order hydrocarbons and oxygenates through the CO/CO2 reduction reaction (CO/CO2RR) at decent selectivity and productivity.

Here, we report a facile approach for synthesizing M–N–C catalysts (M = Co, Fe, Ni) at a commercial scale without employing organic solvents. Our characterization efforts indicate that single atomic catalysts with high surface areas were successfully obtained. Electrochemical measurements demonstrate that, among the three synthesized catalysts, Ni–N–C exhibits the highest performance in the electrochemical CO2 reduction reaction (CO2RR) to carbon monoxide (CO), affording 80% Faradaic efficiency (FE) of CO production at –0.49 VRHE with a turnover frequency (TOF) of 57,379 h–1. Large-scale synthesis coupled with high performance allows moving forward with the practical implementation of M–N–C catalysts for industrially relevant CO2RR.

Amorphous alumina overcoats generated by atomic layer deposition (ALD) have been shown to improve the selectivity and durability of supported metal catalysts in many reactions. Several mechanisms have been proposed to explain the enhanced catalytic performance, but the accessibilities of reactants through the amorphous overcoats remain elusive, which is crucial for understanding reaction mechanisms. Here, we show that an AlO

Electrochemically converting nitrate ions, a widely distributed nitrogen source in industrial wastewater and polluted groundwater, into ammonia represents a sustainable route for both wastewater treatment and ammonia generation. However, it is currently hindered by low catalytic activities, especially under low nitrate concentrations. Here we report a high-performance Ru-dispersed Cu nanowire catalyst that delivers an industrial-relevant nitrate reduction current of 1 A cm

The biggest obstacle to the widespread implantation of polymer electrolyte membrane fuel cells (PEMFCs) is the cost, primarily due to the use of platinum catalysts. The high intrinsic catalyst activity...

Proton exchange membrane fuel cells (PEMFCs) have long been studied for applications in sustainable transportation. The recent shift in focus from passenger vehicle to heavy duty applications places increased demand on the efficiency and durability of the components used in membrane electrode assemblies (MEAs).[1] Of particular interest are the oxygen reduction reaction electrocatalysts used in the fuel cell cathode. While the relaxed capital cost requirements for heavy duty applications allows for increased precious metal loadings, the four-fold increase in operating lifetime requires improved catalysts which can express their high activity not only at beginning-of-life, but also after 25k-hour equivalent accelerated stress tests (ASTs). This paradigm shift prioritizes efforts aimed at understanding and subsequently controlling catalyst degradation. In situ characterization methods can be instrumental in this effort, but it is critical that the operating conditions in these studies reliably replicate the type and degree of degradation observed in the operating fuel cell.[2,3] In this study, identical-location scanning transmission electron microscopy (IL-STEM) is used to compare catalyst degradation in an aqueous environment to degradation observed ex situ in MEAs following AST cycling.[4] For traditional catalysts, the aqueous environment appears to replicate the dissolution and coalescence mechanisms observed for Pt catalysts with small starting particle sizes ( To better replicate the type and degree of degradation in the MEA environment, various experimental parameters such as temperature, acid type/concentration, and upper and lower potential limits were explored. By extending the cycling potential window from 0.6-0.95 Vvs . to 0.4-1.0 Vvs . RHE in an sulfuric acid electrolyte containing Pt ions, the Ostwald ripening mechanism was enhanced, resulting in an end-of-test particle size distribution and composition which better match MEA tests. These refined conditions can now be used to perform in situ and identical-location experiments that will play an important role in the development of robust catalysts for heavy-duty vehicle applications.[6] References [1] D. A. Cullen, et al. Nat. Energy 2021, 6 (5), 462–474. [2] J. A. Gilbert, et al. Electrochim. Acta 2015, 173, 223–234. [3] I. Martens, et al. ACS Energy Lett. 2021, 6 (8), 2742–2749. [4] S. Rasouli, et al. Nano Lett. 2019, 19 (1), 46–53. [5] E. Padgett, et al. J. Electrochem. Soc. 2019, 166 (4), F198–F207 [6] This material is primarily based on work performed by the Million Mile Fuel Cell Truck (M2FCT) Consortium (https://millionmilefuelcelltruck.org), technology manager Greg Kleen, which is supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office. Electron microscopy was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

Aerogels are a very interesting group of materials owing to their unique physical and chemical properties. In the context of electrocatalysis, the focus has been on their physical properties, and they have been used primarily as catalyst supports so far. In this work, we synthesized porphyrin aerogels containing Ni and NiFe mixed metal materials and studied them as catalysts for the oxygen evolution reaction (OER). Different Ni : Fe ratios were synthesized and studied in electrochemical cells, and DFT calculations were conducted in order to gain insight into their behavior. The activity trends were dependent on the metal ratios and differ from known NiFeOOH materials due to the change in the oxidation states of the metals to higher numbers. Herein, we show that Ni and Fe have a synergistic effect on the OER, despite being structurally separated. They are connected electronically, though, through a large organic aromatic system that facilitates electron sharing between them. Among the mixed metal porphyrin aerogels, the best ratio was found to be Ni : Fe = 35 : 65, in contrast to oxide/oxyhydroxide materials in which a ratio of 80 : 20 was found to be ideal.

Anion-exchange membrane electrolyzer cells (AEMECs) are one of the most promising technologies for carbon-neutral hydrogen production. Over the past few years, the performance and durability of AEMECs have substantially improved. Herein, we report an engineered liquid/gas diffusion layer (LGDL) with tunable pore morphologies that enables the high performance of AEMECs. The comparison with a commercial titanium foam in the electrolyzer indicated that the engineered LGDL with thin-flat and straight-pore structures significantly improved the interfacial contacts, mass transport, and activation of more reaction sites, leading to outstanding performance. We obtained a current density of 2.0 A/cm2 at 1.80 V with an efficiency of up to 81.9% at 60 °C under 0.1 M NaOH-fed conditions. The as-achieved high performance in this study provides insight to design advanced LGDLs for the production of low-cost and high-efficiency AEMECs.

We report a strategy to integrate atomically dispersed iron within a heterogeneous nitrogen-doped carbon (N-C) support, inspired by routes for metalation of molecular macrocyclic iron complexes. The N-C support, derived from pyrolysis of a ZIF-8 metal-organic framework, is metalated via solution-phase reaction with FeCl(2) and tributyl amine, as a Brønsted base, at 150 °C. Fe active sites are characterized by (57)Fe Mössbauer spectroscopy and aberration-corrected scanning transmission electron microscopy. The site density can be increased by selective removal of Zn(2+) ions from the N-C support prior to metalation, resembling the transmetalation strategy commonly employed for the preparation of molecular Fe-macrocycles. The utility of this approach is validated by the higher catalytic rates (per total Fe) of these materials relative to established Fe-N-C catalysts, benchmarked using an aerobic oxidation reaction.

Nanoparticles are an important class of materials that exhibit special properties arising from their high surface area-to-volume ratio. Scanning transmission electron microscopy (STEM) has played an important role in nanoparticle characterization, owing to its high spatial resolution, which allows direct visualization of composition and morphology with atomic precision. This typically comes at the cost of sample size, potentially limiting the accuracy and relevance of STEM results, as well as the ability to meaningfully track changes in properties that vary spatially. In this work, automated STEM data acquisition and analysis techniques are employed that enable physical and compositional properties of nanoparticles to be obtained at high resolution over length scales on the order of microns. This is demonstrated by studying the localized effects of potential cycling on electrocatalyst degradation across proton exchange membrane fuel cell cathodes. In contrast to conventional, manual STEM measurements, which produce particle size distributions representing hundreds of particles, these high-throughput automated methods capture tens of thousands of particles and enable nanoparticle size, number density, and composition to be measured as a function of position within the cathode. Comparing the properties of pristine and degraded fuel cells provides statistically robust evidence for the inhomogeneous nature of catalyst degradation across electrodes. These results demonstrate how high-throughput automated STEM techniques can be utilized to investigate local phenomena occurring in nanoparticle systems employed in practical devices.