Electrocatalytic nitrate discount response (NO3RR) is of nice significance for wastewater remediation and ammonia (NH3) synthesis. Nonetheless, environment friendly NO3RR catalysts and a transparent mechanistic understanding are nonetheless missing. Single-atom alloy (SAA) gives a brand new design house for NO3RR with its distinctive atomic and digital buildings. Right here, high-throughput density practical principle (DFT) calculations have been carried out to systematically examine the catalytic potential and response mechanism of Cu-based SAAs for NO3RR to NH3. A volcano relationship between the descriptor ∆E*NO − ∆E*OH and the limiting potential (UL) was established. The outcomes present that Al/Cu (111) achieves an ultra-low UL of −0.18 V. The robust hybridization between Al-p and O-p orbitals permits p electrons to be injected extra readily into anti-bonding orbitals, thereby successfully weakening N-O bond and reducing the response energies of protonation steps. The stronger O affinity of Al website permits Al/Cu (111) to interrupt free from the constraints imposed by standard linear scaling relations and exhibit wonderful NO3RR exercise. Furthermore, Al/Cu (111) protects the lively websites from aggressive H adsorption, resulting in enhanced selectivity. This work establishes p-orbital engineering as a design precept for Cu-based single-atom alloys past standard d-band tuning, offering useful theoretical steerage for NO3RR catalyst design.
