Electrocatalytic CO 2 reduction (CO 2 RR) to valuable fuels is a promising approach to mitigate energy and environmental problems, but controlling the reaction pathways and products remains challenging. Here a novel Cu 2 O nanoparticle film was synthesized by square-wave (SW) electrochemical redox cycling of high-purity Cu foils. The cathode afforded up to 98% Faradaic efficiency for electroreduction of CO 2 to nearly pure formate under ≥45 atm CO 2 in bicarbonate catholytes. When this cathode was paired with a newly developed NiFe hydroxide carbonate anode in KOH/borate anolyte, the resulting two-electrode high-pressure electrolysis cell achieved high energy conversion efficiencies of up to 55.8% stably for long-term formate production. While the high-pressure conditions drastically increased the solubility of CO 2 to enhance CO 2 reduction and suppress hydrogen evolution, the (111)-oriented Cu 2 O film was found to be important to afford nearly 100% CO 2 reduction to formate. The results have implications for CO 2 reduction to a single liquid product with high energy conversion efficiency.
Tuning the facet exposure of Cu could promote the multi-carbon (C2+) products formation in electrocatalytic CO2 reduction. Here we report the design and realization of a dynamic deposition-etch-bombardment method for Cu(100) facets control without using capping agents and polymer binders. The synthesized Cu(100)-rich films lead to a high Faradaic efficiency of 86.5% and a full-cell electricity conversion efficiency of 36.5% towards C2+ products in a flow cell. By further scaling up the electrode into a 25 cm2 membrane electrode assembly system, the overall current can ramp up to 12 A while achieving a single-pass yield of 13.2% for C2+ products. An insight into the influence of Cu facets exposure on intermediates is provided by in situ spectroscopic methods supported by theoretical calculations. The collected information will enable the precise design of CO2 reduction reactions to obtain desired products, a step towards future industrial CO2 refineries.
The electrochemical nitrate reduction reaction (NO 3 RR) on titanium introduces significant surface reconstruction and forms titanium hydride (TiH x , 0 < x ≤ 2). With ex situ grazing-incidence X-ray diffraction (GIXRD) and X-ray absorption spectroscopy (XAS), we demonstrated near-surface TiH 2 enrichment with increasing NO 3 RR applied potential and duration. This quantitative relationship facilitated electrochemical treatment of Ti to form TiH 2 /Ti electrodes for use in NO 3 RR, thereby decoupling hydride formation from NO 3 RR performance. A wide range of NO 3 RR activity and selectivity on TiH 2 /Ti electrodes between −0.4 and −1.0 V RHE was observed and analyzed with density functional theory (DFT) calculations on TiH 2 (111). This work underscores the importance of relating NO 3 RR performance with near-surface electrode structure to advance catalyst design and operation.
Ion exchange (IX) is a promising
technology for selective nitrogen
recovery from urine; however, IX requires chemical-intensive regeneration
that escalates energy consumption and carbon emissions. To overcome
this barrier, we demonstrated and investigated a novel electrified
IX stripping process (EXS) enabling electrochemical in situ IX regeneration with simultaneous ammonia stripping. EXS combines
a weak acid cation exchange resin (WAC) to concentrate ammonia, a
bipolar membrane to produce protons for WAC regeneration, and membrane
stripping to recover the eluted ammonium from WAC. We observed over
80% regeneration (elution from resin) and recovery (membrane stripping)
efficiencies during multiple adsorption–recovery cycles with
synthetic and real urine. Comparing WAC with a strong acid cation
exchange resin illustrated the critical role of the proton affinity
of resin moieties in regulating resin regenerability and conductivity
in EXS, which we distinguished from the rationale for material choice
in electrodeionization. Compared to other electrochemical recovery
methods using unamended wastewater as an electrolyte, EXS enabled
control of electrolyte composition during recovery by separating and
equalizing influent ammonium via WAC-mediated removal. This electrolyte
engineering facilitated tunable EXS energy efficiency (100–300
MJ/kg N). This study informs the design of electrified, intensified
systems that enable decentralized nitrogen recovery from urine.
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