Atomically Dispersed Fe Sites Regulated by Adjacent Single Co Atoms Anchored on N‐P Co‐Doped Carbon Structures for Highly Efficient Oxygen Reduction Reaction

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Abstract

Manipulating the coordination environment and electron distribution for heterogeneous catalysts at the atomic level is an effective strategy to improve electrocatalytic performance but remains challenging. Herein, atomically dispersed Fe and Co anchored on nitrogen, phosphorus co‐doped carbon hollow nanorod structures (FeCo‐NPC) are rationally designed and synthesized. The as‐prepared FeCo‐NPC catalyst exhibits significantly boosted electrocatalytic kinetics and greatly upshifts the half‐wave potential for the oxygen reduction reaction. Furthermore, when utilized as the cathode, the FeCo‐NPC catalyst also displays excellent zinc‐air battery performance. Experimental and theoretical results demonstrate that the introduction of single Co atoms with Co‐N/P coordination around isolated Fe atoms induces asymmetric electron distribution, resulting in the suitable adsorption/desorption ability for oxygen intermediates and the optimized reaction barrier, thereby improving the electrocatalytic activity.

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Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction

Samira Siahrostami, Ambarish R. Kulkarni, Jens K. Nørskov … (2017)

Despite the dedicated search for novel catalysts for fuel cell applications, the intrinsic oxygen reduction reaction (ORR) activity of materials has not improved significantly over the past decade. Here, we review the role of theory in understanding the ORR mechanism and highlight the descriptor-based approaches that have been used to identify catalysts with increased activity. Specifically, by showing that the performance of the commonly studied materials (e.g., metals, alloys, carbons, etc.) is limited by unfavorable scaling relationships (for binding energies of reaction intermediates), we present a number of alternative strategies that may lead to the design and discovery of more promising materials for ORR.

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Engineering bunched Pt-Ni alloy nanocages for efficient oxygen reduction in practical fuel cells

Xinlong Tian, Xiao Xiao Zhao, Ya-Qiong Su … (2019)

Development of efficient and robust electrocatalysts is critical for practical fuel cells. We report one-dimensional bunched platinum-nickel (Pt-Ni) alloy nanocages with a Pt-skin structure for the oxygen reduction reaction that display high mass activity (3.52 amperes per milligram platinum) and specific activity (5.16 milliamperes per square centimeter platinum), or nearly 17 and 14 times higher as compared with a commercial platinum on carbon (Pt/C) catalyst. The catalyst exhibits high stability with negligible activity decay after 50,000 cycles. Both the experimental results and theoretical calculations reveal the existence of fewer strongly bonded platinum-oxygen (Pt-O) sites induced by the strain and ligand effects. Moreover, the fuel cell assembled by this catalyst delivers a current density of 1.5 amperes per square centimeter at 0.6 volts and can operate steadily for at least 180 hours.

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Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

Zhen-Yu Wu, Mohammadreza Karamad, Xue Yong … (2021)

Electrochemically converting nitrate, a widespread water pollutant, back to valuable ammonia is a green and delocalized route for ammonia synthesis, and can be an appealing and supplementary alternative to the Haber-Bosch process. However, as there are other nitrate reduction pathways present, selectively guiding the reaction pathway towards ammonia is currently challenged by the lack of efficient catalysts. Here we report a selective and active nitrate reduction to ammonia on Fe single atom catalyst, with a maximal ammonia Faradaic efficiency of ~ 75% and a yield rate of up to ~ 20,000 μg h −1 mg cat. −1 (0.46 mmol h −1 cm −2 ). Our Fe single atom catalyst can effectively prevent the N-N coupling step required for N 2 due to the lack of neighboring metal sites, promoting ammonia product selectivity. Density functional theory calculations reveal the reaction mechanisms and the potential limiting steps for nitrate reduction on atomically dispersed Fe sites. Developing green and delocalized routes for ammonia synthesis is highly important but still very challenging. Here the authors report an efficient ammonia synthesis process via nitrate reduction to ammonia on Fe single atom catalyst.