Suffering from the competition adsorption between oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), the development of high‐efficiency oxygen electrocatalysts with bifunctional properties still remains a challenge. Herein, a novel and effective neodymium‐evoked valence electronic perturbation strategy to improve and balance reversible oxygen electrocatalysis of metallic cobalt sites is proposed. To heighten the coupling between Nd and Co, the metal‐organic‐framework‐induced method is chosen to prepare the target catalyst of atomic Nd‐doped Co on an N‐doped carbon substrate. The as‐prepared catalyst presents excellent bifunctional electrocatalytic properties with a low overpotential of 288 mV at 10 mA cm−2 for the OER and a high half‐wave potential of 0.85 V for the ORR. The robust electrocatalytic stabilities for both the ORR and OER are also proven. The electrochemical in situ Raman spectra confirm the surface dynamic change of the transformation of oxygen intermediates by noting the formation of Co–OOH. Theoretical calculations verify that the adsorption of oxygen intermediates is balanced owing to the strong Co 3d‐Nd 4f orbital electronic coupling effect below the Fermi level. Moreover, the potential practicability of catalyst is further demonstrated in solid‐state rechargeable Zn‐Air batteries, which exhibit large power density and a long cycling life.

Neodymium‐Evoked Valence Electronic Modulation to Balance Reversible Oxygen Electrocatalysis

Cobalt single atom anchored on N-doped carbon nanoboxes as typical single-atom catalysts (SACs) for boosting the overall water splitting

The growth of renewable energy industries and the ongoing need for fertilizer in agriculture have created a need for sustainable production of ammonia (NH3) using low-cost, environment-friendly techniques. The electrocatalytic nitrate (NO3-) reduction reaction (NO3RR) has the potential to improve both the management of environmental nitrogen and the recycling of synthetic nutrients. However, NO3RR is frequently hindered by the incomplete NO3- conversion, sluggish reaction kinetics, and suppression of the hydrogen evolution reaction (HER). Inspired by specific local electronic structures that are adjustable for single-atom catalysts, this work presents a nanohybrid electrocatalytic filter with iron single atoms (FeSA) immobilized on MXene. The fabricated FeSA/MXene filter exhibited maximum NH3 Faradaic efficiency and selectivity (82.9 and 99.2%, respectively) that were higher than those for filters made of Fe nanoparticles anchored on MXene (FeNP/MXene) (69.2 and 81.3%, respectively) and MXene alone (32.8 and 52.4%, respectively), measured at an initial pH of 7 and an applied potential of -1.4 V vs Ag/AgCl. Density functional theory calculations revealed that, compared to the FeNP/MXene filter, the FeSA/MXene filter prevented the competition from the HER and reduced the activation energy of the potential-limiting step (*NO to *NHO) that made the NH3 synthesis thermodynamically favorable . This work highlights an alternative strategy for achieving a synergistic NO3- removal and nutrient recovery with durable catalytic activity and stability.

Fluidic MXene Electrode Functionalized with Iron Single Atoms for Selective Electrocatalytic Nitrate Transformation to Ammonia.

The low intrinsic catalytic performance and stability are the two dominant obstacles for alkaline hydrogen evolution reaction (HER) electrocatalyst. Herein, amorphous molybdenum oxide (MoOx) has been introduced to rhodium hierarchical nanosheets (MoOxRh-HNS) at atomic level efficiently reducing the barrier for hydrogen spillover from Rh to MoOx; thereby, MoOxRh-HNS exhibit superior HER activity with mass activity of 23.9 A mgnoble metal−1 at overpotential of 200 mV, which is boosted by 10.8- and 14.9-fold with relative to Rh-HNS and Pt/C in alkaline media, respectively. Meanwhile, Tafel slope is as low as 22.5 mV dec−1 for MoOxRh-HNS revealing a hydrogen-spillover-involving HER mechanism proved by the electrochemical test as well as operando electrochemical impedance spectroscopy. Density functional theory calculation indicates the adsorbed hydrogen on MoOxRh promotes the water dissociation and balances the hydrogen binding strength to a moderate level. Simultaneously, the hierarchical nanosheet structure contributes a robust HER stability at 500 mA cm−2. This work offers a new methodology to construct a high-performance alkaline HER electrocatalyst with industrial-level current density. 

Hydrogen spillover in MoOxRh hierarchical nanosheets boosts alkaline HER catalytic activity

Abstract Water splitting, an efficient technology to produce purified hydrogen, normally requires high cell voltage (>1.5 V), which restricts the application of single atoms electrocatalyst in water oxidation due to the inferior stability, especially in acidic environment. Substitution of anodic oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) effectually reduces the overall voltage. In this work, the utilization of iridium single atom (Ir‐SA/NC) as robust hydrogen evolution reaction (HER) and HzOR electrocatalyst in 0.5 m H2SO4 electrolyte is reported. Mass activity of Ir‐SA/NC is as high as 37.02 A mgIr −1 at overpotential of 50 mV in HER catalysis, boosted by 127‐time than Pt/C. Besides, Ir‐SA/NC requires only 0.39 V versus RHE to attain 10 mA cm−2 in HzOR catalysis, dramatically lower than OER (1.5 V versus RHE); importantly, a superior stability is achieved in HzOR. Moreover, the mass activity at 0.5 V versus RHE is enhanced by 83‐fold than Pt/C. The in situ Raman spectroscopy investigation suggests the HzOR pathway follows *N2H4→*2NH2→*2NH→2N→*N2→N2 for Ir‐SA/NC. The hydrazine assisted water splitting demands only 0.39 V to drive, 1.25 V lower than acidic water splitting.

Hydrazine-Assisted Acidic Water Splitting Driven by Iridium Single Atoms.

The commercialization of rechargeable zinc air batteries (ZABs) requires the discovery of high-performance, low-cost and durable bifunctional oxygen electrocatalysts. In this work, we report nitrogen doped carbon nano/microtubes confined metallic cobalt nanoparticles and single atoms ([email protected]/[email protected]) as robust oxygen electrocatalyst for rechargeable ZABs. [email protected]/[email protected] exhibits 18 times better ORR performance than [email protected] ascribed to the relay catalysis by Co-SAs and Co-NPs via O2→H2O2→H2O pathway. Experimental and theoretical investigations reveal that Co-SAs are capable of efficient oxygen reduction to H2O2, which is further reduced to H2O by Co-NPs due to its higher oxophilicity. Besides, due to the formed microtubes, the overpotential at 100 mA cm−2 in OER catalysis is lowered by 130 mV for [email protected]/[email protected] than [email protected] The power density of the assembled rechargeable ZAB is 155 mW cm−2 for [email protected]/[email protected] outperforming the noble-metal counterpart (Pt/CB-IrO2: 71 mW cm−2). Furthermore, a superior stability with inappreciable increment in voltage gap for 300 h is achieved. [email protected]/[email protected] also performs its high potential in the practical application with a maximum battery performance of 120 mW cm−2 sustained for 17 h in all-solid-state ZABs test. 

Co single atoms and Co nanoparticle relay electrocatalyst for rechargeable zinc air batteries

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Co single atoms and Co nanoparticle relay electrocatalyst for rechargeable zinc air batteries