According to Yang Shao-Horn's principle, CoSe2 is a promising candidate as an efficient, affordable, and sustainable alternative electrocatalyst for the oxygen evolution reaction, owing to its well-suited electronic configuration of Co ions. However, the catalytic efficiency of pure CoSe2 is still far below what is expected, because of its poor active site exposure yield. Herein, we successfully overcome the disadvantage of insufficient active sites in bulk CoSe2 by reducing its thickness into the atomic scale rather than any additional modification (such as doping or hybridizing with graphene or noble metals). The positron annihilation spectrometry and XAFS spectra provide clear evidence that a large number of VCo″ vacancies formed in the ultrathin nanosheets. The first-principles calculations reveal that these VCo″ vacancies can serve as active sites to efficiently catalyze the oxygen evolution reaction, manifesting an OER overpotential as low as 0.32 V at 10 mA cm(-2) in pH 13 medium, which is superior to the values for its bulk counterparts as well as those for the most reported Co-based electrocatalysts. Considering the outstanding performance of the simple, unmodified ultrathin CoSe2 nanosheets as the only catalyst, further improvement of the catalytic activity is expected when various strategies of doping or hybridizing are used. These results not only demonstrate the potential of a notable, affordable, and earth-abundant water oxidation electrocatalyst based on ultrathin CoSe2 nanosheets but also open up a promising avenue into the exploration of excellent active and durable catalysts toward replacing noble metals for oxygen electrocatalysis.
Nitrate is ar aw ingredient for the production of fertilizer,g unpowder,a nd explosives.D eveloping an alternative approach to activate the NNbond of naturally abundant nitrogen to form nitrate under ambient conditions will be of importance.Herein, pothole-rich WO 3 was used to catalyse the activation of N Nc ovalent triple bonds for the direct nitrate synthesis at room temperature.T he pothole-rich structure endues the WO 3 nanosheet more dangling bonds and more easily excited high momentum electrons,w hicho vercome the two major bottlenecks in NNb ond activation, that is,p oor binding of N 2 to catalytic materials and the high energy involved in this reaction. The average rate of nitrate production is as high as 1.92 mg g À1 h À1 under ambient conditions,without any sacrificial agent or precious-metal co-catalysts.M ore generally,t he concepts will initiate an ew pathwayf or triggering inert catalytic reactions.
Versatile catalyst systems with large current density under industrial conditions are pivotal to give impetus to hydrogen energy from fundamental to practical applications. Herein, a Schottky heterojunction nanosheet array composed of dispersed NiFe hydroxide nanoparticles and ultrathin NiS nanosheets (NiFe LDH/NiS) is proposed to regulate cooperatively mass transport and electronic structure for triggering oxygen evolution reaction (OER) activity at high current. In catalytic systems, the rich porosity of the NiS nanosheet array contributes abundant catalytic sites and good infiltration of the electrolyte for fast mass transfer. Furthermore, theoretical calculations reveal the coupling of NiFe LDH onto the NiS could tune the d‐band center of Ni(Fe) atoms and the binding strength of oxygen intermediates for favorable OER kinetics. Therefore, the NiFe LDH/NiS Schottky heterojunction exhibits a remarkable OER activity, delivering a current density of 1000 mA cm–2 at the ultralow overpotential of 325 mV. Meanwhile, scaled‐up NiFe LDH/NiS electrodes are implemented in an industrial water splitting electrolyzer and exhibit a stable cell voltage of 2.01 V to deliver a constant catalytic current of 8000 mA over 80 h, saving 0.215 kWh of electricity to generate more hydrogen per cubic meter than commercial Raney Ni electrodes.
Development of efficient and affordable electrocatalysts in neutral solutions is paramount importance for the renewable energy.Herein, we report that the oxygen evolution reaction (OER) performance of Co 3 S 4 under neutral conditions can be enhanced by exposed octahedral planes and selfadapted spin states in atomically thin nanosheets.AHAADF image clearly confirmed that the active octahedra with JahnTeller distortions were exposed exclusively.M ost importantly, in the atomically thin nanosheets,the spin states of Co 3+ in the octahedral self-adapt from low-spin to high-spin states.A s aresult, the synergistic effect endow the Co 3 S 4 nanosheets with superior OER performance,w ith exceptional low onset overpotentials of circa 0.31 Vinneutral solutions,which is state-ofthe-art among inorganic non-noble metal compounds.
Tandem catalysts can divide the reaction into distinct steps by local multiple sites and thus are attractive to trigger CO2RR to C2+ products. However, the evolution of catalysts generally exists during CO2RR, thus a closer investigation of the reconstitution, interplay, and active origin of dual components in tandem catalysts is warranted. Here, taking AgI−CuO as a conceptual tandem catalyst, we uncovered the interaction of two phases during the electrochemical reconstruction. Multiple operando techniques unraveled that in situ iodine ions leaching from AgI restrained the entire reduction of CuO to acquire stable active Cu0/Cu+ species during the CO2RR. This way, the residual iodine species of the Ag matrix accelerated CO generation and iodine‐induced Cu0/Cu+ promotes C−C coupling. This self‐adaptive dual‐optimization endowed our catalysts with an excellent C2+ Faradaic efficiency of 68.9 %. Material operando changes in this work offer a new approach for manipulating active species towards enhancing C2+ products.
BackgroundPerioperative systemic steroid administration for rapid recovery in total knee and hip arthroplasty (TKA/THA) is an important and controversial topic. We conducted this systematic review and meta-analysis to evaluate the overall benefits and harms of perioperative systemic steroid in patients undergoing TKA and THA.MethodsA comprehensive search was performed on PubMed, OVID, and Web of Science databases, and a systematic approach was carried out starting from the PRISMA recommendations. Relevant randomized controlled trials (RCTs) were selected. The risk of bias was evaluated according to the Cochrane Handbook for Systematic Reviews of Interventions version. Data were extracted and meta-analyzed or qualitatively synthesized for all the outcomes.ResultsData were extracted from 11 trials involving 774 procedures. Meta-analysis showed that high-dose systemic steroid (dexamethasone > 0.1 mg/kg) rather than low dose is effective to reduce postoperative nausea and vomiting and postoperative acute pain (within 24 h). In addition, systemic steroid is associated within faster functional rehabilitation and greater inflammation control. On the other hand, systemic steroid is associated with a higher level of postoperative serum glucose on the operation day. The complications between groups are similarly low.ConclusionsOur study suggests that by providing lower incidence of postoperative nausea and vomiting and less postoperative acute pain, high-dose systemic steroid plays a critical role in rapid recovery to TKA and THA. The preliminary results also show the superior possibility of systemic steroid in functional rehabilitation and inflammation control. More large, high-quality studies that investigate the safety and dose–response relationship are necessary.Electronic supplementary materialThe online version of this article (doi:10.1186/s13018-017-0601-4) contains supplementary material, which is available to authorized users.
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