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B, N-Co Doped Porous Carbon Nanotubes Supported Cu Single Atoms and B-Doped Cu Nanoparticles for High-Performance Electrocatalytic NO3RR and Zn-Nitrate Batteries
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DOI：10.1002/cey2.70313.png)
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Abstract
En 中文
Electrocatalytic nitrate reduction (NO3RR) is a green, environmentally benign, and energy-efficient approach to ammonia synthesis; however, it is hampered by the competing hydrogen evolution reaction (HER) and complex electron/proton transfer pathways, which lead to low selectivity and sluggish kinetics. Herein, a hierarchical catalyst, denoted as B-Cu NPs/BNC, was constructed by co-anchoring Cu single atoms (Cu–N/C) and B-doped Cu nanoparticles (B–Cu) onto B, N co-doped porous carbon nanotubes. Comprehensive structural characterizations (XRD, HRTEM, and XAFS) confirmed that interstitial B doping increased the Cu–Cu bond length and lattice spacing, whereas XPS and DFT calculations revealed that the introduction of Cu nanoparticles and B doping induced strong interfacial coupling between Cu atoms and the carbon substrate while regulating the local electronic structures of both Cu single atoms and Cu nanoparticles. As a result, the Cu d-band center was upshifted, which optimized the adsorption and activation of key intermediates, altered the rate-determining step, and lowered the corresponding energy barrier. These electronic modulations were found to reduce the energy barrier of the rate-determining step, suppress side reactions, and inhibit the HER, thereby improving the selectivity toward NH3. Consequently, the optimal B-Cu NPs/BNC-7 catalyst delivered exceptional NO3RR performance, achieving a maximum NH3 yield of 14.95 mg h−1 cm−2 at −0.9 V versus RHE and a peak Faradaic efficiency of 92.8% at −0.6 V versus RHE in an alkaline electrolyte. Furthermore, when assembled as the cathode in a Zn-nitrate battery, the catalyst delivered a power density of 18.86 mW cm−2 with excellent cycling stability.
Keywords:
B-doped Cu nanoparticles
Cu single atoms
electrocatalytic nitrate reduction porous carbon nanotubes
zinc-nitrate batteries
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