Palladium has been recognized as the best anodic, monometallic electrocatalyst for the formic acid oxidation (FAO) reaction in a direct formic acid fuel cell. Here we report a systematic study of FAO on a variety of Pd nanocrystals, including cubes, right bipyramids, octahedra, tetrahedra, decahedra, and icosahedra. These nanocrystals were synthesized with approximately the same size, but different types of facets and twin defects on their surfaces. Our measurements indicate that the Pd nanocrystals enclosed by {1 0 0} facets have higher specific activities than those enclosed by {1 1 1} facets, in agreement with prior observations for Pd single‐crystal substrates. If comparing nanocrystals predominantly enclosed by a specific type of facet, {1 0 0} or {1 1 1}, those with twin defects displayed greatly enhanced FAO activities compared to their single‐crystal counterparts. To rationalize these experimental results, we performed periodic, self‐consistent DFT calculations on model single‐crystal substrates of Pd, representing the active sites present in the nanocrystals used in the experiments. The calculation results suggest that the enhancement of FAO activity on defect regions, represented by Pd(2 1 1) sites, compared to the activity of both Pd(1 0 0) and Pd(1 1 1) surfaces, could be attributed to an increased flux through the HCOO‐mediated pathway rather than the COOH‐mediated pathway on Pd(2 1 1). Since COOH has been identified as a precursor to CO, a site‐poisoning species, a lower coverage of CO at the defect regions will lead to a higher activity for the corresponding nanocrystal catalysts, containing those defect regions.

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Exploring durable electrocatalysts with high activity for oxygen evolution reaction (OER) in acidic media is of paramount importance for H2 production via polymer electrolyte membrane electrolyzers, yet it remains urgently challenging. Herein, we report a synergistic strategy of Rh doping and surface oxygen vacancies to precisely regulate unconventional OER reaction path via the Ru–O–Rh active sites of Rh-RuO2, simultaneously boosting intrinsic activity and stability. The stabilized low-valent catalyst exhibits a remarkable performance, with an overpotential of 161 mV at 10 mA cm−2 and activity retention of 99.2% exceeding 700 h at 50 mA cm−2. Quasi in situ/operando characterizations demonstrate the recurrence of reversible oxygen species under working potentials for enhanced activity and durability. It is theoretically revealed that Rh-RuO2 passes through a more optimal reaction path of lattice oxygen mediated mechanism-oxygen vacancy site mechanism induced by the synergistic interaction of defects and Ru–O–Rh active sites with the rate-determining step of *O formation, breaking the barrier limitation (*OOH) of the traditional adsorption evolution mechanism.

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We report the observation of efficient charge-to-spin conversion in the three-dimensional topological insulator (TI) Bi2Se3 and Ag bilayer by the spin-torque ferromagnetic resonance technique. The spin orbit torque ratio in the Bi2Se3/Ag/CoFeB heterostructure shows a significant enhancement as the Ag thickness increases to ~2 nm and reaches a value of 0.5 for 5 nm Ag, which is ~3 times higher than that of Bi2Se3/CoFeB at room temperature. The observation reveals the interfacial effect of Bi2Se3/Ag exceeds that of the topological surface states (TSS) in the Bi2Se3 layer and plays a dominant role in the charge-to-spin conversion in the Bi2Se3/Ag/CoFeB system. Based on the first-principles calculations, we attribute our observation to the large Rashba-splitting bands which wrap the TSS band and has the same net spin polarization direction as TSS of Bi2Se3.Subsequently, we demonstrate for the first time the Rashba induced magnetization switching in Bi2Se3/Ag/Py with a low current density of 5 5.8 10  A/cm 2 .

This unique and comprehensive introduction offers an unrivalled and in-depth understanding of the computational-based thermodynamic approach and how it can be used to guide the design of materials for robust performances, integrating basic fundamental concepts with experimental techniques and practical industrial applications, to provide readers with a thorough grounding in the subject. Topics covered range from the underlying thermodynamic principles, to the theory and methodology of thermodynamic data collecting, analysis, modeling, and verification, with details on free energy, phase equilibrium, phase diagrams, chemical reactions, and electrochemistry. In thermodynamic modelling, the authors focus on the CALPHAD method and first-principles calculations. They also provide guidance for use of YPHON, a mixed-space phonon code developed by the authors for polar materials based on the supercell approach. Including worked examples, case studies, and end-of-chapter problems, this is an essential resource for students, researchers, and practitioners in materials science.

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