Published: July 1, 2024
Language: Английский
Desalination, Journal Year: 2024, Volume and Issue: 586, P. 117884 - 117884
Published: June 29, 2024
Language: Английский
Citations
12
ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(8), P. 3887 - 3912
Published: July 17, 2024
Language: Английский
Citations
9
JACS Au, Journal Year: 2025, Volume and Issue: 5(3), P. 1221 - 1231
Published: Feb. 27, 2025
Homogeneous platinum catalysts for hydrosilylation are essential the chemical industry and society, through production of commodities such as functional silicones. However, high boiling points products low concentration homogeneous make implementation traditional separation methods difficult. Catalyst loss becomes a core sustainability techno-economic challenge. In addition, highly active platinum-based have remarkable susceptibility to deactivation upon reaction completion. Recently, redox-mediated electrosorption has been successfully demonstrated in number electrically conductive media platform. industrial systems carried out nonconductive media. Therefore, developing an electrochemical recycling system realistic, can be transformative sustainable catalysis manufacturing. Here, we overcome these challenges catalyst by introducing strongly coordinating vinyl ligand enabling Pt solvent-free, nonpolar reactant two distinct loops electrosorbent regeneration. The olefin maintains catalytic activity after prevents particle aggregation, primary mechanism deactivation. stabilized coordinated reversibly adsorbed released electrosorbent, demonstrating 100% retention over 90% release efficiency. A analysis supports economic potential system, with cost savings >5k USD/kgPt. By combining design engineering, demonstrate industrially relevant practical
Language: Английский
Citations
1
Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(25), P. 15006 - 15018
Published: Jan. 1, 2024
Redox-electrodes are designed to selectively bind platinum group metals by auto-oxidation, and release them electrochemically. The platform can efficiently recover PGMs from catalytic converter leachates, contribute energy-efficient technologies for materials recycling.
Language: Английский
Citations
4
ACS ES&T Engineering, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 28, 2025
Language: Английский
Citations
0
Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown
Published: April 2, 2025
Electrified interfaces are critical to the performance of energy systems and often demonstrate substantial complexity under operating conditions. A nanoscale understanding interfacial microenvironment, i.e., solid-electrolyte interphase (SEI), in lithium-mediated nitrogen reduction (Li-N2R) is key for realizing efficient ammonia (NH3) production. Herein, we used time-resolved neutron reflectometry (NR) observe SEI formation Li-N2R We found that LiBF4-based electrolyte provided a substantially more well-defined layer than previous NR interrogations LiClO4, highlighting underlying chemistry dictates design enabling new NR-based studies. Using situ NR, LiBF4-derived conditions comprises thick, diffuse outer thin, compact inner at low current cycling (<2 mA/cm2), revealing structure which ex studies have not been able probe. Increased sustained led merging layers into single-layer SEI. isotope contrast methods with d6-EtOH d8-THF drive tracking growth cycling, proton donor modifies layer, solvent layer. Li dendritic was observed absence donor. Neutron absorption also indicated presence boron SEI, underscoring value neutron-based interrogation. Our results inform Li-based reaction microenvironments, these can be applied broadly technologies.
Language: Английский
Citations
0
The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(16), P. 4444 - 4450
Published: April 16, 2024
Neutron reflectometry has long been a powerful tool to study the interfacial properties of energy materials. Recently, time-resolved neutron used better understand transient phenomena in electrochemical systems. Those measurements often comprise large number reflectivity curves acquired over narrow q range, with each individual curve having lower information content compared typical steady-state measurement. In this work, we present an approach that leverages existing reinforcement learning tools model data extract time evolution structure parameters. By mapping taken at different times as states, use Soft Actor-Critic algorithm optimize series parameters best represent system. We show constitutes elegant solution modeling data.
Language: Английский
Citations
3
Published: Nov. 25, 2024
Electrified interfaces are critical to the performance of energy systems and often demonstrate substantial complexity under operating conditions. Nanoscale understanding interfacial microenvironment, i.e., solid electrolyte interphase (SEI), in lithium-mediated nitrogen reduction (Li-N2R) is key for realizing efficient ammonia (NH3) production. Herein, we have used time-resolved neutron reflectometry (NR) observe SEI formation Li-N2R We found that LiBF4-based provided a substantially more well-defined layer than previous NR interrogation LiClO4, highlighting underlying chemistry dictates design enabling new NR-based studies. Using situ reflectometry, LiBF4-derived conditions comprises thick, diffuse outer thin, compact inner at low current cycling (<2 mA/cm2), revealing structure which ex studies not been able probe. Increased sustained led merge layers single-layer SEI. isotope contrast methods with d6-EtOH d8-THF drive tracking growth cycling, proton donor modifies layer, solvent layer. Li dendritic was observed absence donor. Neutron absorption also indicated presence boron SEI, underscoring value neutron-based interrogation. Our results inform Li-based reaction microenvironments, these can be applied broadly technologies.
Language: Английский
Citations
1
ACS Physical Chemistry Au, Journal Year: 2024, Volume and Issue: 4(6), P. 615 - 619
Published: Sept. 3, 2024
Of the attributes that determine performance of electroactive film-based devices, least well quantified and understood is spatial distribution component species. This critical since it dictates transport rates all mobile species (electrons, counterions, solvent, analyte, reactant) film mechanical properties (as exploited in actuator devices). One few techniques able to provide individual population profiles situ specular neutron reflectivity (NR). Historically, this information obtained at cost poor time resolution (hours). Here we show how NR measurements with event mode data acquisition enable both temporal resolution; latter can be selected postexperiment varied during transient. We profile "buried" interfaces under dynamic electrochemical conditions polypyrrole electrodeposition Cu deposition/dissolution. In case polypyrrole, homogeneous throughout growth; there no evidence dendrite formation followed by solvent (water) displacement. Correlation NR-derived thickness coulometric assay allows calculation volume fraction, ϕS = 0.48. a deep eutectic complexing nature medium results time-dependent metal speciation: mechanistically, dissolution does not simply follow deposition pathway reverse.
Language: Английский
Citations
0
Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 504, P. 158537 - 158537
Published: Dec. 11, 2024
Language: Английский
Citations
0