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1.
ACS Sustain Chem Eng ; 12(3): 1185-1194, 2024 Jan 22.
Article in English | MEDLINE | ID: mdl-38273987

ABSTRACT

While plastic pollution threatens ecosystems and human health, the use of plastic products continues to increase. Limiting its harm requires design strategies for plastic products informed by the threats that plastics pose to the environment. Thus, we developed a sustainability metric for the ecodesign of plastic products with low environmental persistence and uncompromised performance. To do this, we integrated the environmental degradation rate of plastic into established material selection strategies, deriving material indices for environmental persistence. By comparing indices for the environmental impact of on-the-market plastics and proposed alternatives, we show that accounting for the environmental persistence of plastics in design could translate to societal benefits of hundreds of millions of dollars for a single consumer product. Our analysis identifies the materials and their properties that deserve development, adoption, and investment to create functional and less environmentally impactful plastic products.

2.
ACS Appl Mater Interfaces ; 13(49): 58682-58690, 2021 Dec 15.
Article in English | MEDLINE | ID: mdl-34860485

ABSTRACT

A two-stage ball milling process was used to synthesize amorphous Ni79.2Nb12.5Y8.3 and Ni74.2Co5Nb12.5Y8.3 nanoparticles from elemental powders. The two-stage ball milling process provides a scalable and industrially applicable method for producing non-metalloid amorphous nanoparticles. The amorphous nanoparticles displayed excellent catalytic performance toward the oxygen evolution reaction (OER) in 1 M KOH, displaying lower overpotentials than IrO2 at 10 mA cm-2. The addition of Co in the amorphous alloy reduced the overpotential to 288 mV at 10 mA cm-2. The pairing of X-ray photoelectron spectroscopy and in situ X-ray absorption spectroscopy revealed that the improved OER activity of amorphous Ni74.2Co5Nb12.5Y8.3 was attributed to the catalytic synergy between Y and Co. The integration of Y supported proton-coupled electron-transfer processes that assisted with the electrostatic adsorption of OH- and formation of oxyhydroxide species, while Co sites enabled metal-oxo bonding to prevent Ni overcharging and the stabilization of ß-NiOOH. The catalytic synergy between Y and Co reduces the amount of Co needed to enhance the OER activity of Ni-based alloys and lessens the dependence on Co, which is in high demand in many renewable energy and storage applications.

3.
Adv Mater ; 33(45): e2103812, 2021 Nov.
Article in English | MEDLINE | ID: mdl-34541731

ABSTRACT

The oxygen evolution reaction (OER) limits the energy efficiency of electrocatalytic systems due to the high overpotential symptomatic of poor reaction kinetics; this problem worsens over time if the performance of the OER electrocatalyst diminishes during operation. Here, a novel synthesis of nanocrystalline Ni-Co-Se using ball milling at cryogenic temperature is reported. It is discovered that, by anodizing the Ni-Co-Se structure during OER, Se ions leach out of the original structure, allowing water molecules to hydrate Ni and Co defective sites, and the nanoparticles to evolve into an active Ni-Co oxyhydroxide. This transformation is observed using operando X-ray absorption spectroscopy, with the findings confirmed using density functional theory calculations. The resulting electrocatalyst exhibits an overpotential of 279 mV at 0.5 A cm-2 and 329 mV at 1 A cm-2 and sustained performance for 500 h. This is achieved using low mass loadings (0.36 mg cm-2 ) of cobalt. Incorporating the electrocatalyst in an anion exchange membrane water electrolyzer yields a current density of 1 A cm-2 at 1.75 V for 95 h without decay in performance. When the electrocatalyst is integrated into a CO2 -to-ethylene electrolyzer, a record-setting full cell voltage of 3 V at current density 1 A cm-2 is achieved.

4.
Science ; 367(6478): 661-666, 2020 02 07.
Article in English | MEDLINE | ID: mdl-32029623

ABSTRACT

Electrolysis offers an attractive route to upgrade greenhouse gases such as carbon dioxide (CO2) to valuable fuels and feedstocks; however, productivity is often limited by gas diffusion through a liquid electrolyte to the surface of the catalyst. Here, we present a catalyst:ionomer bulk heterojunction (CIBH) architecture that decouples gas, ion, and electron transport. The CIBH comprises a metal and a superfine ionomer layer with hydrophobic and hydrophilic functionalities that extend gas and ion transport from tens of nanometers to the micrometer scale. By applying this design strategy, we achieved CO2 electroreduction on copper in 7 M potassium hydroxide electrolyte (pH ≈ 15) with an ethylene partial current density of 1.3 amperes per square centimeter at 45% cathodic energy efficiency.

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