Abundant Dislocation Layered Double Hydroxides Synthesis by Molten Salt with Bound Water Boosting Oxygen Evolution

Abstract

Recently, great effort has been applied to explore non-noble metal catalysts. However, the ambiguous understanding of active transfer mechanisms hinders the electrocatalysts design. [6][7][8] It has been reported that the appropriate design of the crystal distortion can improve catalytic performance for the modulated electronic structure of the active site. [9][10][11] Nevertheless, in the past, all the strategies focused on replacing the element of octahedron with others, which was inevitable for the change of intrinsic electronic structure caused by the introduction of other elements. [12,13] Meanwhile, most studies have focused on analyzing electronic structures while the contribution of structural changes for the generation of active phases is ignored chronically. [14][15][16] In fact, the active phase generated during the electrochemical process is considered to be the truly electrochemically active substance. [3,17,18] Besides, the coexistence of octahedral and tetrahedral in oxides such as spinel and chalcocite also limits further understanding of the accurate catalytic mechanism. [19,20] Notably, introducing strain not only generates the inner strain energy promoting the active phase transformation but also can tune the distortion degree of octahedral, thereby modulating their electronic structure and catalytic properties. [21] It is interesting to note that layered double hydroxides (LDHs) are composed entirely of octahedral. [22][23][24] Hence, the intrinsic effects of octahedral deformation can be well analyzed to help the development of advanced electrocatalysts. Moreover, it has excellent intrinsic activity comparable to precious metals, including RuO 2 and IrO 2 .Firstly, we use the density functional theory (DFT) calculations to reveal that tensile stress modifies the electronic structure. The distribution of e g and t 2g electrons was changed and the d band center was enhanced, optimizing adsorption energy and promoting OER process. Despite this, there remain many obstacles to introducing strain into the LDHs. As a kind of hydroxide, LDHs are very fragile and very easy to destroy in the process of producing internal stress. Dislocations have stress fields that are capable of generating the required tensile stress to modulate the catalytic performance and are able to modulate the catalytic performance (Figures S1 and S2, Supporting Information). Therefore, strain energy can be introduced by

Integrating Sub‐Nano Catalysts into Metal‐Organic Framework toward Pore‐Confined Polysulfides Conversion in Lithium‐Sulfur Batteries

“…Metal-organic frameworks (MOFs), constructed by diversified metal clusters and customizable ligands, can be theoretically served as multifunctional sulfur hosts for their porosity, diverse structures, and chemical designability. [22][23][24][25][26][27][28][29][30][31] Most MOFs, such as ZIF-8, UiO-66, MIL-101(Cr), PCN-224, MIL-100, HKUST-1, et.al, have been applied as sulfur hosts. [32][33][34] However, the state of art porous MOF hosts mainly focus on the storage of sulfur inside the porous structure and constraining the diffusion of sulfur species through physical-chemical interaction between framework and polysulfides.…”

Recent Advances on Transition‐Metal‐Based Layered Double Hydroxides Nanosheets for Electrocatalytic Energy Conversion

“…CoV-LDHs 1 m KOH 250 @ 10 44 [58] NiFe-LDHs 1 m KOH 270 @ 10 48.6 [59] NiFe-LDHs-MPs 1 m KOH 250 @ 100 34.5 [51] NiFe-LDHs 1 m KOH 324 @ 10 57.4 [60] CoNi-LDHs-E 1 m KOH 280 @ 10 81 [61] Ta-NiFe LDHs 1 m KOH 260 @ 50 58.95 [62] D-NiFe LDHs 1 m KOH 199 @ 10 26.9 [52] NiFe LDHs/Co 1−x S 1 m KOH 251 @ 10 41.67 [63] NiFeV-LDHs 1 m KOH 195 @ 20 42 [64] NiFe III (1:1)-LDHs 1 m KOH 183 @ 10 31.1 [65] NiCo 1 Fe 1 -LDHs 1 m KOH 231 @ 10 59 [66] CoVRu-LDHs 1 m KOH 263 @ 25 74.5 [53] Fe-NiV-LDHs 1 m KOH 255 @ 10 56 [67] NiFeV-LDHs 1 m KOH 224 @ 10 32.7 [68] NiFeNb-0.25-LDHs 1 m KOH 277 @ 100 50.6 [69] NiFeCo-LDHs 1 m KOH 249 @ 10 42 [70] v-NiFe-LDHs 1 m KOH 195 @ 10 47.9 [71] EE-NiFe-LDHs 1 m KOH 205 @ 10 41.8 [72] NiCoFe-LDHs 1 m KOH 174 @ 10 50 [73] NiFe-LDHs-V Ni 1 M KOH 229 @ 10 62.9 [74] v-NiFe-LDHs 1 m KOH 150 @ 10 37.1 [75] D-NiFeZn-LDHs 0.1 m KOH 200 @ 20 34.9 [54] NiFe-LDHS-V O 1 m KOH 230 @ 10 39.6 [76] D-CoFe-LDHs 1 m KOH 283 @ 10 39 [77] MnNiFe-LDHs-laser 1 m KOH 220 @ 10 37 [78] M-NiFe-LDHs 1 m KOH 217 @ 10 45.1 [79] AGC/MnCo-LDHs 1 m KOH 370 @ 10 127.5 [80] Co-C@NiFe-LDHs 1 m KOH 249 @ 10 57.9 [56] FeNi-LDHs/CoP 1 m KOH 231@ 20 33.5 [81] FeCoNi-LDHs/CuO/Cu 1 m KOH 243.1 @ 50 63.8 [57] FeNi 2 Se 4 -FeNi-LDHs 1 m KOH 205 @ 10 30.14 [55] MIM-CoFe-LDHs 1 m KOH 216.8@10 39.3 [82] CoNi-LDHs/Ti 3 C 2 T x 1 m KOH 200 @ 50 68 [83] CoNi-LDHs@PCPs 1 m KOH 350 @ 10 58 [84] Ni 3 S 2 /Cu-NiCo-LDHs 1 m KOH 119 @ 10 70 [85] NiCo-LDHs/NiCoS 1 m KOH 308@ 100 48 …”

“…Afterward, abundant dislocations are validated to promote the OER active phase formation of NiFe-LDHs nanosheets. [52] Compare with pristine NiFe-LDHs nanosheets, the overpotential of NiFe-LDHs nanosheets with ample dislocations at 10 mA cm −2 was reduced from 223 to 199 mV, manifesting the positive influence of dislocation on OER performance.…”

Lattice‐Strain Engineering for Heterogenous Electrocatalytic Oxygen Evolution Reaction

“…In this review, we present a thorough overview of the newest achievements in various types of lattice-strain engineering in OER and summarize theoretical calculations and modeling of strain effects as well as experimental progress. As illustrated in Figure 1, we will methodically elucidate the strain-reactivity correlations in four modules: [74][75][76][77][78][79][80][81][82][83][84] i) fundamental mechanisms; ii) strain strategies; iii) electrocatalysts; iv) identification techniques. Finally, we discuss and outlook the perspective applications of lattice-strain engineering in different electrocatalytic fields, including ORR, HER, NRR, and ECO 2 RR, simultaneously presenting novel insight into the drawbacks.…”

“…Copyright 2021, American Chemical Society. ii) Reproduced with permission [75]. Copyright 2022, Wiley-VCH.…”