Electrocatalysis plays a decisive role in various energy-related applications Engineering the active sites of electrocatalysts is an important aspect to promote their catalytic performance In particular, defect engineering provides a feasible and efficient approach to improve the intrinsic activities and increase the number of active sites in electrocatalysts In this review, recent investigations on defect engineering of a wide range of electrocatalysts such as metal-free carbon materials, transition metal oxides, transition metal dichalcogenides and metal-organic frameworks (MOFs) will be summarized Different defect creation strategies will be outlined, for example, heteroatom doping and removal, plasma irradiation, hydrogenation, amorphization, phase transition and reduction treatment In addition, we will overview the commonly used advanced characterization techniques that could confirm the existence and identify the detailed structures, types and concentration of defects in electrocatalysts The defect characterization tools are beneficial for gaining an in-depth understanding of defects on electrocatalysis and thus could reveal the structure-performance relationship Finally, the major challenges and future development directions on defect engineering of electrocatalysts will be discussed

Defect engineering and characterization of active sites for efficient electrocatalysis

The early stages of nucleation and growth of dislocations by irradiation in urania is clarified based on the combination of experiments and atomistic calculations. It is established that irradiation induced dislocations follow a five stage process: (i) point defects are first created by irradiation, (ii) they aggregate into clusters, (iii) from which nucleate Frank loops, (iv) which transform into unfaulted loops via Shockley that in turn grow, and (v) finally reorganize into forest dislocations. Stages (i)–(iii) participate in the lattice expansion while the onset of lattice contraction starts with stage (iv), i.e., when unfaulted loops nucleate. Irradiation induced dislocations operate in the spontaneous recombination regime, to be opposed to the thermal diffusion regime. Body of arguments collaborates to this statement, the main one is the comparison between characteristic distances estimated from the dose rate (Vat/(K0×τ))13 and from the diffusion coefficient  (D×τ)12. Such a comparison identifies materials under irradiation as belonging either into the recombination regime or not.

Early stages of irradiation induced dislocations in urania

Ion accelerators have been used by material scientists for decades to investigate radiation damage formation in nuclear materials and thus to emulate neutron-induced changes. The versatility of conditions in terms of particle energy, dose rate, fluence, etc., is a key asset of ion beams allowing for fully instrumented analytical studies. In addition, very short irradiation times and handling of non-radioactive samples dramatically curtail the global cost and duration as compared to in-reactor testing. Coupling of two or more beams, use of heated/cooled sample holders, and implementation of in situ characterization and microscopy pave the way to real time observation of microstructural and property evolution in various extreme radiation conditions more closely mimicking the nuclear environments. For these reasons, multiple ion beam facilities have been commissioned worldwide. In France, under the auspices of the Universite Paris-Saclay, the JANNuS platform for ‘Joint Accelerators for Nanosciences and Nuclear Simulation’ comprises five ion implanter and electrostatic accelerators with complementary performances. At CSNSM (CNRS & Univ Paris-Sud, Orsay), a 200 kV Transmission Electron Microscope is coupled to an accelerator and an implanter for in situ observation of microstructure modifications induced by ion beams in a material, making important contribution to the understanding of physical phenomena at the nanoscale. At CEA Paris-Saclay, the unique triple beam facility in Europe allows the simultaneous irradiation with heavy ions (like Fe, W) for nuclear recoil damage and implantation of a large array of ions including gasses for well-controlled modelling-oriented experiments. Several classes of materials are of interest for the nuclear industry ranging from metals and alloys, to oxides or glasses and carbides. This paper gives selected examples that illustrate the use of JANNuS ion beams in investigating the radiation resistance of structural materials for today’s and tomorrow’s nuclear reactors.

Investigating radiation damage in nuclear energy materials using JANNuS multiple ion beams

Extended defect change in UO2 during in situ TEM annealing

TEM characterization of dislocation loops in proton irradiated single crystal ThO2

Evolution of extended defects in polycrystalline Au-irradiated UO2 using in situ TEM: Temperature and fluence effects

Influence of exogenous xenon atoms on the evolution kinetics of extended defects in polycrystalline UO2 using in situ TEM

Full characterization of dislocations in ion-irradiated polycrystalline UO2

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Evolution of extended defects in polycrystalline Au-irradiated UO2 using in situ TEM: Temperature and fluence effects

Influence of exogenous xenon atoms on the evolution kinetics of extended defects in polycrystalline UO2 using in situ TEM

Full characterization of dislocations in ion-irradiated polycrystalline UO2