This review provides an overview of electrocatalytic reduction of nitrate, including the reaction mechanisms, reactor design principles, product detection methods, and performance evaluation methods, which can provide a sustainable nitrogen cycle.
Hydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. Here we theoretically profile that the interfacial charge accumulation induces by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ show a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivers the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.
Electrochemical carbon dioxide (CO 2 )r eduction reaction (CO 2 RR) is an attractive approach to deal with the emission of CO 2 and to produce valuable fuels and chemicals in ac arbon-neutral way.M any efforts have been devoted to boost the activity and selectivity of high-value multicarbon products (C 2+ )o nC u-based electrocatalysts.H owever,C ubased CO 2 RR electrocatalysts suffer from poor catalytic stability mainly due to the structural degradation and loss of active species under CO 2 RR condition. To date,most reported Cu-based electrocatalysts present stabilities over dozenso f hours,w hich limits the advance of Cu-based electrocatalysts for CO 2 RR. Herein, ap orous chlorine-doped Cu electrocatalyst exhibits high C 2+ Faradaic efficiency (FE) of 53.8 %at À1.00 Vv ersus reversible hydrogen electrode (V RHE ). Importantly,the catalyst exhibited an outstanding catalytic stability in long-term electrocatalysis over 240 h. Experimental results show that the chlorine-induced stable cationic Cu 0 /Cu + species and the well-preserved structure with abundant active sites are critical to the high FE of C 2+ in the long-term run of electrochemical CO 2 reduction.
Pristine
Ru generally shows unsatisfying activity for the electrocatalytic
hydrogen evolution reaction (HER). How to activate its HER activity
through facile methodologies is very challenging. Recently, metal-supported
electrocatalysts integrating metals with efficient hydrogen adsorption
and supports with facile hydrogen desorption delivered a high HER
performance through a metal-to-support hydrogen spillover process,
where the small metal–support work function difference (ΔΦ)
was identified as the criterion for the successful interfacial hydrogen
spillover. Herein, we demonstrate that a hydrogen spillover strategy
significantly boosts the HER activity of Ru by depositing a Ru1Fe1 alloy on CoP (Ru1Fe1/CoP)
with a small ΔΦ of 0.05 eV. Experimentally, Ru1Fe1/CoP (0.7 wt % Ru loading) delivered a high Ru utilization
activity of 139.8 A/mgRu and a long-term durability in
acid. Mechanism investigations authenticated that the small ΔΦ
guaranteed the interfacial hydrogen spillover from Ru1Fe1 with efficient hydrogen adsorption to CoP with facile hydrogen
desorption and thereafter boosted the HER activity of Ru.
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