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Selective Electrochemical Reduction of CO₂ to Metal Oxalates in Nonaqueous Solutions Using Trace Metal Pb on Carbon Supports Enhanced by a Tailored Microenvironment

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Advanced Energy Materials 2025年

作者： Brower, Rowan S. Wuille Bille, Brian Chiu, Shawn Perryman, Joseph T. Yao, Libo Agboola, Faridat O. Nagasaka, Cocoro A. Xie, Yinuo Gomez-Caballero, Richard Kumari, Ankita Neumann, Elizabeth K. Alexandrova, Anastassia N. McCrory, Charles C. L. Velázquez, Jesus M. Department of Chemistry University of California-Davis Davis 95616 CA United States Department of Chemistry and Biochemistry University of California-Los Angeles Los Angeles 90095-1569 CA United States Department of Chemical Engineering University of Michigan Ann Arbor 48109 MI United States Department of Chemistry University of Michigan Ann Arbor 48109-1055 MI United States Department of Chemistry Universidad de Puerto Rico Recinto de Río Piedras San Juan PR 00931-3346 Puerto Rico Macromolecular Science & Engineering Program University of Michigan Ann Arbor 48109-2102 MI United States

In this work, the electroreduction of carbon dioxide (CO2) to oxalate is enabled by incorporating trace metallic lead (Pb) on carbon-based supports (CBS) with polymer overlayers. These composite materials serve as an ... 详细信息

In this work, the electroreduction of carbon dioxide (CO₂) to oxalate is enabled by incorporating trace metallic lead (Pb) on carbon-based supports (CBS) with polymer overlayers. These composite materials serve as an efficient electrocatalytic system for the facile conversion and storage of CO₂, a pernicious atmospheric pollutant. Results from controlled potential electrolysis experiments indicate that 1) trace metallic Pb on the ppb scale is active toward the reductive coupling of CO₂ to oxalate at comparable Faradaic efficiencies to bulk metallic Pb and 2) polymer encapsulation of this trace metallic Pb leads to promotion of CO₂ reduction (CO₂R) selectively to metal oxalates over other products such as CO. Importantly, metal oxalates are important alternative cementitious materials and precursors for other materials’ synthesis applications. The solid products undergo rigorous spectroscopic characterization, including ¹³CO₂ labeling experiments, to ensure the metal oxalates are in fact produced from CO₂R. These findings serve as a model for leveraging microenvironment effects to enhance activity and selectivity for CO₂R using trace-metal catalysts for carbon utilization and storage technologies. © 2025 The Author(s). Advanced Energy Materials published by Wiley-VCH GmbH.

关键词： alternative cementitious materials carbon capture and utilization carbon dioxide reduction catalyst microenvironment trace metal

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Bioimmobilization using huisgen -dipolar cycloaddition on vapor-based polymer coatings

Bioimmobilization using huisgen -dipolar cycloaddition on va...

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235th ACS National Meeting, Spring 2008

作者： Nandivada, Himabindu Jiang, Xuwei Panades, Augusti Bourke, Allison Yoshida, Mutsumi Chen, Hsien-Yeh Lahann, Joerg Macromolecular Science and Engineering Program Department of Chemical Engineering University of Michigan 2300 Hayward St. Ann Arbor MI 48109-2136 United States

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Spatially controlled engineering of biointerfaces via functionalized poly-p-xylylenes

Spatially controlled engineering of biointerfaces via functi...

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235th ACS National Meeting, Spring 2008

作者： Chen, Hsien-Yeh Jiang, Xuwei Yoshida, Mutsumi Lahann, Joerg Macromolecular Science and Engineering Program Department of Chemical Engineering University of Michigan 2300 Hayward St. Ann Arbor MI 48109-2136 United States

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Erratum: “The scaling of zero-shear viscosities of semidilute polymer solutions with concentration” [J. Rheol. 49, 1117–1128 (2005)]

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Journal of Rheology 2007年第5期51卷 1099-1100页

作者： Youngsuk Heo Ronald G. Larson Macromolecular Science and Engineering Program University of Michigan Ann Arbor Michigan 48109 Department of Chemical Engineering and Macromolecular Science and Engineering Program University of Michigan Ann Arbor Michigan 48109

Page 1124. For three distinct polymer-solvent pairs, namely polystyrene in benzene, polyisoprene in cyclohexane, and polybutadiene in cyclohexane, we erroneousl

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Nonlinear viscoelasticity of native and engineered ligament and tendon

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2010 Annual Conference on Experimental and Applied Mechanics

作者： Jinjin, Ma. Arruda, Ellen M. Department of Mechanical Engineering University of Michigan United States Department of Biomedical Engineering University of Michigan United States Macromolecular Science and Engineering Program University of Michigan United States

ISBN: (纸本)9781441994974

Ligaments and tendons are non-linear viscoelastic materials and their response functions are typically assessed using creep and stress relaxation tests. Non-linear viscoelastic models such as multiple Maxwell elements in parallel and the quasilinear viscoelastic model (QLV) used to capture the non-linear viscoelastic response of ligaments and tendons frequently employ multiple relaxation time constants determined from curve-fitting the entire available data set and generally lack a clear physiological relevance. Uniaxial load-unload tension tests on ligament and tendon also manifests the viscoelastic response and such experiments suggest that the bulk of the non-linearity in the response of these soft tissues is in the elasticity. We propose physiologically relevant nonlinear viscoelastic models in which the response of the main structural proteins in ligament and tendon (e.g. collagen and elastin) are described using non-linear elasticity. Our approach using a three-element, non-linear solid micromechanical model captures this viscoelastic response in load-unload, stress relaxation and creep with a limited number of physically meaningful parameters. Previous research also shows different viscoelastic responses between native tendon and ligaments. In our model, by varying the properties of the non-linear springs, we are able to capture the differences in the viscoelastic responses of ligaments verses tendon. We will demonstrate the capabilities of our model by comparing to the experimental results from testing native and engineered ligament and tendon. ©2010 Society for Experimental Mechanics Inc.

关键词： Tendons

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Gradient sequence π-conjugated copolymers

Gradient sequence π-conjugated copolymers

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作者： Palermo, Edmund F. McNeil, Anne J. Department of Chemistry and Macromolecular Science and Engineering Program University of Michigan 930 North University Avenue Ann ArborMI48109-1055 United States

ISBN: (纸本)9780841230019

Gradient sequence copolymers exhibit a gradual change in comonomer composition along the polymer chain. These novel materials are interesting because they exhibit unique properties compared to their random, alternating and block copolymer counterparts. We describe herein the synthesis and characterization of the first π-conjugated gradient sequence copolymers, which have only recently been accessible via a controlled, chain-growth synthetic method. We demonstrate that the gradient sequence copolymers exhibit unique thermal, optical and morphological properties compared to the analogous block and random copolymers. In addition, we show that gradient sequence copolymers can act as additives to modulate the thin film morphologies and phase separation behavior of polymer/polymer and polymer/fullerene blends. The impact of gradient sequence copolymer-based additives in stabilizing bulk heterojunction organic solar cells is also described. © 2014 American Chemical Society.

关键词： Phase separation

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Functional surface modification of anisotropic biphasic nanoparticles for selective cell targeting

Functional surface modification of anisotropic biphasic nano...

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8th World Biomaterials Congress 2008, WBC 2008

作者： Yoshida, Mutsumi Roh, Kyung-Ho Lahann, Joerg Department of Chemical Engineering University of Michigan Ann Arbor MI United States Macromolecular Science and Engineering Program University of Michigan Ann Arbor MI United States

ISBN: (纸本)9781615670802

Biocompatibility of biphasic particles supports their use in biomedical applications. With the added capability of selectively targeting cells with directionality and controlled orientation, the biphasic nanocolloids may serve as a flexible platform requiring complex, multifunctionality, as both compartments can be independently loaded as well as be surface-modified to control orientation relative to the cell surface. Taken together these properties of anisotropic biphasic nanocolloids may enable capabilities such as self-assembly into three-dimensional tissue constructs or mimicry of subcellular organization which may not be achievable with more conventional, isotropic nanoparticles.

关键词： Nanoparticles

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Short-term biocompatibility of functionalized polymer coatings made by chemical vapor deposition polymerization

Short-term biocompatibility of functionalized polymer coatin...

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8th World Biomaterials Congress 2008, WBC 2008

作者： Yoshida, Mutsumi Elkasabi, Yaseen Lahann, Joerg Department of Chemical Engineering University of Michigan Ann Arbor MI United States Macromolecular Science and Engineering Program University of Michigan Ann Arbor MI United States

ISBN: (纸本)9781615670802

CVD polymerization of functionalized [2.2]paracyclophanes provides a generalized, simple process by which multiple reactivity can be afforded on various substrates with a range of geometry or topology. In addition, this method provides controllable ratios of presented functional groups and minimizes cross-reactivity of biomolecules as immobilization can be done in sequence. Initial assessment of biocompatibility of CVD coatings underscore the importance of controlled ratio of surface-presented functional groups, as small differences in the chemical composition of co-polymers can have significant impact in cellular response.

关键词： Biocompatibility

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Crystallization of POSS in a PEG-based multiblock polyurethane: Toward a hybrid hydrogel

Crystallization of POSS in a PEG-based multiblock polyuretha...

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2004 Materials Research Society Fall Meeting

作者： Wu, Jian Ge, Qing Burke, Kelly A. Mather, Patrick T. Polymer Program Institute of Materials Science University of Connecticut Storrs CT 06269-3136 Department of Macromolecular Science and Engineering Case Western Reserve University Cleveland OH 44106

Building upon earlier success in forming materials with crystalline ordering of POSS via the telechelic architecture with POSS end-capping polyethylene glycols, here we report similar ordering in PEG-POSS thermoplastic polyurethane applicable to a novel hybrid hydrogel. Thus, a unique series of hybrid thermoplastic polyurethanes (TPUs) were synthesized using poly(ethylene glycol) (PEG) as soft segment and incorporating an isobutyl-functionalized POSS diol (TMP POSS diol) in the hard segment. The molecular weight of PEG was systematically varied to include 10: 20, and 35 kDa while the mole ratio of PEG to POSS diol (as chain extender) was chosen as 8:1. The diisocyanate employed for TPU polymerization was 4,4'methylenebis(phenyl-isocyanate) (MDI). Wide-angle X-ray diffraction (WAXD) studies revealed that both the hydrophilic soft segments (PEG) and hydrophobic hard segments (POSS) can form crystalline structures driven by micro-phase separation, itself due to thermodynamic incompatibility. Differential scanning calorimetry (DSC) and rheological studies revealed that thermal history is important in controlling the crystallization of a POSS-rich nanophase. Increasing the cooling rate monotonically decreases the crystallinity of POSS-rich phase and results in a decrease in the ultimate dynamic storage modulus following POSS crystallization and an increase of the loss angle for temperatures above Tm of PEG and below Tm of POSS. We conclude that both composition and thermal history are key factors in determing the internal network built by the POSS nanophase, which will have a significant influence on the properties of the resulting hybrid hydrogels now being studied. © 2005 Materials Research Society.

关键词： Crystallization

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Microfluidic actuation system based on electrolysis of ionic liquid/water

Microfluidic actuation system based on electrolysis of ionic...

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13th International Conference on Miniaturized Systems for Chemistry and Life sciences, MicroTAS 2009

作者： Tung, Yi-Chung Takayama, Shuichi Department of Biomedical Engineering University of Michigan United States Research Center for Applied Sciences Academia Sinica Taiwan Macromolecular Science and Engineering Program University of Michigan United States

ISBN: (纸本)9780979806421

This paper reports a novel fully-disposable, cost-effective microfluidic actuation system requires no fluidic interfacing, and minimal electric connections. The device is constructed of multiple polydimethylsiloxane (PDMS) layers and a glass substrate. Taking advantage of the unique material properties of ionic liquids (IL), the device has long shelf life (> 48 hours) and can be fully functioned in high humidity environments. The microfluidic single and multiple valve and pump devices are demonstrated in the paper. The developed system provides a promising actuation scheme for point-of-care μTAS used in the field. © 2009 CBMS.

关键词： Ionic liquids

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