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One of the challenges in polymer electrolyte membrane fuel cells (PEMFCs) is developing cost‐effective, active and stable catalyst for oxygen reduction reaction (ORR). Platinum alloy‐based catalyst materials have drawn great attention and been intensively investigated for the excellent activity property, with some of them already exceeding 2020 DOE target for the ORR activity. In the meantime, the electrochemical stability of these Pt alloys remains a challenge to be overcome. This review first highlights important understandings of ORR pathways and mechanisms and then proceeds to summarize recent research progresses on development of Pt alloy catalyst materials. Current obstacles in Pt alloy catalyst research are discussed, with the stability issue being specifically emphasized and a theoretical model being developed for depicting the stability property. This review also provides perspectives of future research directions in this field.

 

Understanding the growth pathway of faceted alloy nanoparticles at the atomic level is crucial to morphology control and property tuning. Yet, it remains a challenge due to complexity of the growth process and technical limits of modern characterization tools. We report a combinational use of multiple cutting-edge in situ techniques to study the growth process of octahedral Pt₃Ni nanoparticles, which reveal the particle growth and facet formation mechanisms. Our studies confirm the formation of octahedral Pt₃Ni initiates from Pt nuclei generation, which is followed by continuous Pt reduction that simultaneously catalyzes Ni reduction, resulting in mixed alloy formation with moderate elemental segregation. Carbon monoxide molecules serve as a facet formation modulator and induce Ni segregation to the surface, which inhibits the (111) facet growth and causes the particle shape to evolve from a spherical cluster to an octahedron as the (001) facet continues to grow.

 

Oxygen evolution reaction (OER) is of great significance for hydrogen production via water electrolysis, which, however, demands development of highly active, durable, and cost‐effective electrocatalysts in order to stride into a renewable energy era. Herein, highly efficient and long‐term durable OER by coupling B and P into an amorphous porous NiFe‐based electrocatalyst is reported, which possesses an amorphous porous metallic bulk structure and high corrosion resistance, and overcomes the issues associated with currently used catalyst nanomaterials. The PB codoping in the activated NiFePB (a‐NiFePB) delocalizes both Fe and Ni at Fermi energy level and enhances p–d hybridization as simulated by density functional theory calculations. The harmonized electronic structure and unique porous framework of the a‐NiFePB consequently improve the OER activity. The activated NiFePB thus exhibits an extraordinarily low overpotential of 197 mV for harvesting 10 mA cm⁻²OER current density and 233 mV for reaching 100 mA cm⁻²under chronopotentiometry condition, with the Tafel slope harmoniously conforming to 34 mV dec⁻¹. Impressive long‐term stability of this new catalyst is evidenced by only limited activity decay after 1400 h operation at 100 mA cm⁻². This work strategically directs a way for heading up a promising energy conversion alternative.

 

Capacitive deionization (CDI) is an energy saving and environmentally friendly technology for water desalination. However, classical CDI is challenged by a low salt removal capacity. To improve the desalination capacity, electrode materials utilizing the battery mechanism for salt ion removal have emerged as a new direction more recently. In this work, we report a study of amorphous iron phosphate (FePO 4 ) as a promising electrode material for pseudocapacitive sodium ion removal. Sodium ions can be effectively, reversibly intercalated and de-intercalated upon its electrochemical reduction and oxidation, with an excellent sodium ion capacity under half-cell testing conditions. By assembling a hybrid CDI (HCDI) system utilizing the FePO 4 electrode for pseudocapacitive sodium ion removal and active carbon electrode for capacitive chloride ion removal, the cell exhibited a high salt removal capacity and good reversibility and durability, which was attributed to the advantageous features of amorphous FePO 4 . The HCDI system achieved a high deionization capacity (82 mg g −1 ) in 10 mM NaCl, a fast deionization rate (0.046 mg g −1 s −1 ), and good stability and cyclability. 

Formaldehyde is an essential building block for hundreds of chemicals and a promising liquid organic hydrogen carrier (LOHC), yet its indirect energy-intensive synthesis process prohibits it from playing a more significant role. Here we report a direct CO reduction to formaldehyde (CORTF) process that utilizes hydrogen underpotential deposition to overcome the thermodynamic barrier and the scaling relationship restriction. This is the first time that this reaction has been realized under ambient conditions. Using molybdenum phosphide as a catalyst, formaldehyde was produced with nearly a 100% faradaic efficiency in aqueous KOH solution, with its formation rate being one order of magnitude higher compared with the state-of-the-art thermal catalysis approach. Simultaneous tuning of the current density and reaction temperature led to a more selective and productive formaldehyde synthesis, indicating the electrochemical and thermal duality of this reaction. DFT calculations revealed that the desorption of the *H 2 CO intermediate likely served as the rate-limiting step, and the participation of H 2 O made the reaction thermodynamically favorable. Furthermore, a full-cell reaction set-up was demonstrated with CO hydrogenation to HCHO achieved without any energy input, which fully realized the spontaneous potential of the reaction. Our study shows the feasibility of combining thermal and electrochemical approaches for realizing the thermodynamics and for scaling relationship-confined reactions, which could serve as a new strategy in future reaction design.