RESUMO
Defects have been found to enhance the electrocatalytic performance of NiFe-LDH for oxygen evolution reaction (OER). Nevertheless, their specific configuration and the role played in regulating the surface reconstruction of electrocatalysts remain ambiguous. Herein, cationic vacancy defects are generated via aprotic-solvent-solvation-induced leaking of metal cations from NiFe-LDH nanosheets. DFT calculation and in situ Raman spectroscopic observation both reveal that the as-generated cationic vacancy defects tend to exist as VM (M=Ni/Fe); under increasing applied voltage, they tend to assume the configuration VMOH , and eventually transform into VMOH-H which is the most active yet most difficult to form thermodynamically. Meanwhile, with increasing voltage the surface crystalline Ni(OH)x in the NiFe-LDH is gradually converted into disordered status; under sufficiently high voltage when oxygen bubbles start to evolve, local NiOOH species become appearing, which is the residual product from the formation of vacancy VMOH-H . Thus, we demonstrate that the cationic defects evolve along with increasing applied voltage (VM â VMOH â VMOH-H ), and reveal the essential motif for the surface restructuration process of NiFe-LDH (crystalline Ni(OH)x â disordered Ni(OH)x â NiOOH). Our work provides insight into defect-induced surface restructuration behaviors of NiFe-LDH as a typical precatalyst for efficient OER electrocatalysis.
RESUMO
Eutrophication and acidification have been the most concerned environmental problems in coastal ecosystem. However, their combined effect on coastal ecosystem function was unknown. Both diatom (Conticribra weissflogii) and dinoflagellate (Prorocentrum donghaiense) are used as coastal algal model. Seven parameters were determined for physiological function assessment, including cell density, chlorophyll a (Chl a), protein, malonaldehyde (MDA), superoxide dismutase, carbonic anhydrase (CA), and nitrate reductase (NR). The influence of nitrate (N) and phosphate (P) on MDA and CA in C. weissflogii was significant, and that on Chl a and protein in P. donghaiense were also significant. However, the influence of acidification on physiological functions was not significant. The effect of acidification could be intensified by coastal eutrophication. More importantly, the coexist influence of acidification and eutrophication on CA, NR and protein in C. weissflogii and MDA in P. donghaiense was significant. Both NR activity and Chl a content in P. donghaiense were positively correlated to N and P concentration when pH were 7.9 and 7.8, respectively. With simultaneous worsening of acidification and eutrophication, the cell growth of P. Donghaiense was accelerated more obviously than C. weissflogii, i.e., dinoflagellate was more adaptable than diatom, thus algal species distribution and abundance could be changed.
