Electrochemically in-situ generation of oxygen and caustic soda is promising for sulfide management while suffers from scaling, poor inactivating capacity, hydrogen release and ammonia escape. In this study, the four-compartment electrochemical cell efficiently captured oxygen molecules from the air chamber to produce HO without generating toxic by-products. Meanwhile, the catalyst layer surface of PTFE/CB-GDE maintained a relatively balanced gas-liquid micro-environment, enabling the formation of enduring solid-liquid-gas interfaces for efficient HO electrosynthesis. A dramatic increase in HO generation rate from 453.3 mg L h to 575.4 mg L h was attained by advancement in operation parameters design (flow channels, electrolyte types, flow rates and circulation types). Stability testing resulted in the HO generation rate over 15 g L and the current efficiency (CE) exceeding 85%, indicating a robust stable operational capacity. Furthermore, after 120 mg L HO treatment, an increase of 11.1% in necrotic and apoptotic cells in the sewer biofilm was observed, higher than that achieved with the addition of NaOH, HO method. The in-situ electrosynthesis strategy for HO represents a significance toward the practical implementation of sulfide abatement in sewers, holding the potential to treat various sulfide-containing wastewater.
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http://dx.doi.org/10.1016/j.jhazmat.2024.134181 | DOI Listing |
Angew Chem Int Ed Engl
December 2024
University of Toronto - St George Campus: University of Toronto, Department of Electrical and Computer Engineering, CANADA.
The electrochemical reduction of CO2 to CH4 is promising for carbon neutrality and renewable energy storage but confronts low CH4 selectivity, especially at high current densities. The key challenge lies in promoting *CO intermediate and *H coupling while minimizing side reactions including C-C coupling or H-H coupling, which is particularly difficult at high current density due to abundant intermediates. Here we report a cooperative strategy to address this challenge using Cu-based catalysts comprising Cu-N coordination polymer and CuO component that can simultaneously manage the key intermediates *CO and *H.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
City University of Hong Kong, Department of Chemistry, Tat Chee Avenue, 000000, Kowloon, HONG KONG.
Electrocatalytic CO2 reduction (CO2R) to multi-carbon (C2+) products in strong acid presents a promising approach to mitigate the CO2 loss commonly encountered in alkaline and neutral systems. However, this process often suffers from low selectivity for C2+ products due to the competing C1 (e.g.
View Article and Find Full Text PDFSmall
December 2024
Department of Chemical Engineering, National Cheng Kung University, Tainan City, 70101, Taiwan.
Development of high-performance and inexpensive electrocatalysts for oxygen evolution reaction (OER) at neutral pH is important for direct seawater splitting and organic electrosynthesis but remains challenging due to the sluggish OER kinetics and diverse side reactions inherent to the constituents of working electrolytes. Herein, we report on a P:NiFe electrode, containing P-doped NiFe alloy, as an excellent electrocatalyst for hydrogen evolution reaction (HER) and OER pre-catalyst for efficient OER in both seawater and organic electrolyte for adiponitrile (ADN) electrosynthesis at neutral pH. Fe and P species modulate the coordination environment of nickel sites, which enables the simultaneous formation of OER-active nickel species and FePO passivation layer, thus transforming HER-active P:NiFe to OER-active a-P:NiFe.
View Article and Find Full Text PDFSmall
December 2024
Department of Chemical Engineering, Queen's University, Kingston, ON, K7L 3N6, Canada.
Electrochemical carbon dioxide (CO) reduction from aqueous solutions offers a promising strategy to overcome flooding and salt precipitation in gas diffusion electrodes used in gas-phase CO electrolysis. However, liquid-phase CO electrolysis often exhibits low CO reduction rates because of limited CO availability. Here, a macroporous Ag mesh is employed and activated to achieve selective CO conversion to CO with high rates from an aqueous bicarbonate solution.
View Article and Find Full Text PDFAdv Mater
December 2024
School of Materials Science and Engineering, Peking University, Beijing, 100871, P. R. China.
Renewable electricity-driven CO electroreduction provides a promising route toward carbon neutrality and sustainable chemical production. Nevertheless, the viability of this route faces constraints of catalytic efficiency and durability in near-neutral electrolytes at industrial-scale current densities, mechanistically originating from unfavorable accommodation of H species from water dissociation. Herein, a new strategy is reported to accelerate water dissociation by the rich surface hydroxyl on bismuth subcarbonate nanosheets in situ electrochemical transformed from bismuth hydroxide nanotube precursors.
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