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Xiao et al. Microstructures 2023;3:2023006  https://dx.doi.org/10.20517/microstructures.2022.26  Page 13 of 17

               systems exhibit complex structures and substantial compositional constitutions, which could significantly
               influence hydrogen diffusion and the associated mechanical responses. Therefore, the effects of structures
               (i.e., phase structures, vacancies and dislocations) and constitutions (substitutional and interstitial atoms) in
               HEAs on hydrogen-induced mechanical behavior and the underlying mechanisms should be carefully
               studied. Notably, a quantitative model has been proposed by Nag et al. and Kamachali et al., which
               demonstrated that the solute-solute interactions and internal stresses can significantly affect the
               thermodynamic properties and strengthening mechanisms of HEA systems [78,79] . If the H atoms are
               incorporated into the HEAs with highly-diverse chemistries, the effects of complex chemistry on the
               mechanical responses and deformation mechanisms in the HEAs with H atoms should be experimentally
               and theoretically carried out. The role of complex chemistry in the formation of “surfaces” in crack
               formation and propagation also needs to be explored.

               (2) As earlier demonstrated, hydrogen atoms are preferentially partitioned into GBs and then reduce the
               cohesive strength of GBs. Therefore, the structural features of GBs play a key role in determining the HE
               resistance of alloys. Based on this, it could be an effective routine to achieve enhanced HE resistance in
               HEAs via elaborately designing the GB architectures (e.g., introducing precipitates at GBs and creating GB
               segregation). Therefore, further research should be focused on the innovative design of novel GB structures
               in the HEAs.

               (3) For HE-resistant materials, hydrogen local concentration is a critical parameter in governing the
               resistance to HE. When exposed to hydrogen environments for sufficient durations, a low hydrogen
               concentration stems basically from low hydrogen solubility and sluggish hydrogen diffusion in most
               metallic alloy systems. Therefore, the effect of a specific element on hydrogen solubility and hydrogen
               diffusion in different HEA systems should be systematically investigated. We believe that studies along this
               direction could help to significantly accelerate the design of HEAs that are intrinsically resistant to HE.

               (4) It is well known that atomic-scale microstructural traps can substantially limit hydrogen diffusion. For
               instance, Chen et al. showed that hydrogen can be trapped in the core of finely dispersed V-Mo-Nb carbides
                            [30]
               in ferritic steels . Furthermore, it was also reported that hydrogen concentration is observed at carbon-rich
                                                                                            [80]
               dislocations and incoherent interfaces between niobium carbides and the surrounding steel . Therefore, it
               could be an effective strategy to enhance the resistance to HE in HEAs via engineering hydrogen traps, i.e.,
                                                                           [81]
               nanoscale  carbides  and  low-energy  dislocation  nanostructures . In  addition,  state-of-the-art
               microstructural characterization techniques like cryogenic atom probe tomography should be employed to
               directly observe the hydrogen distribution of HEA systems.


               (5) Similar to Ni-based superalloys, L1 -strengthened HEAs have shown significant promise in high-
                                                  2
               temperature applications. However, it has been recognized that oxygen-assisted GB damage plays an
               important role in the ITE issue. Therefore, improving oxidation resistance may be an efficient avenue that
               can hinder the oxygen-accelerated GB damage. Furthermore, as earlier reported, serrated GBs and
               columnar-like grains can effectively address the ITE issues. It should be noted that such unique GB
               structures can greatly reduce the diffusion kinetics of the oxygen and then delay intergranular cracking. As a
               result, careful tailoring of GB features should be carried out to further improve the resistance to ITE in
               HEAs. In contrast, it has been recognized that creating hydrogen traps and reducing diffusion kinetics can
               effectively improve the resistance to HE. We expect that L1 -strengthened HEAs with unique GB features
                                                                  2
               are also highly HE resistant, owing to the suppressed diffusion kinetics (serrated GBs and columnar-like
               grains) and high-density hydrogen traps (L1 /matrix interfaces).
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