promising alternative to fossil fuels. Water electrolysis by renewable resourcederived electricity represents a facile and green route to produce H 2. [1-13] Generally, the key to implement high-performance water splitting is to develop economically viable, efficient, and robust electrocatalysts to lower the activation potential barriers. Thus far, researchers have devoted extensive enthusiasm to the investigation of electrocatalysts. Currently, most efforts have been taken on the search for new materials, [14-16] regulation of morphology, [17] crystallinity, [18] facet, [19] component, [20-24] defect, [25,26] matter phase, [27,28] or the compositing of various materials with synergy. [29-36] However, the performances of emerging nonnoble electrocatalysts still lag behind those of noble ones. To address this issue, researchers have turned their attention beyond the electrocatalysts themselves. Field-assisted electrocatalysis is the electrocatalytic reaction proceeded in the presence of a field. It represents a promising methodology since it exerts an additional degree of freedom to engineer an electrochemical process. Inspiringly, indisputable improvements in electrocatalytic hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) have been implemented with the assist of various fields, including electric field, magnetic field, strain, and light. For example, the electrocatalytic HER of a MoS 2 nanosheet is markedly boosted by simply exploiting a back gate voltage of 5 V. [37] Its overpotential at −100 mA cm −2 is decreased from 240 to 38 mV. In addition, enhancement of alkaline water electrolysis is achieved by applying a moderate magnetic field (≤450 mT) to an electrocatalytic anode consists of highly magnetic electrocatalysts. [38] Its current density increments are beyond 100%. Furthermore, the HER activity of β-PdH x increases monotonically as the applied strain increases from 0% to 4.5%. [39] Lastly, an approximately threefold increase in current density of Au-MoS 2 for electrocatalytic HER is realized upon the illumination of IR light. [40] These results undoubtedly elucidate that applying a field during electrocataly sis opens up great opportunities toward further improving electrocatalytic activity. Moreover, this approach provides merits of facile, dynamical, continuous, reversible, and universal control. Despite fascinating achievements, these investigations are relatively scattered. The underneath mechanisms and principles Hydrogen fuel is considered as one of the most clean renewable resources, warranting it a primary alternative to fossil fuels for future energy supplies. Electrocatalytic water splitting is an eco-friendly technique for high-purity hydrogen production. However, the sluggish dynamics of its two halfreactions, hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), are tough challenges impeding the practical application of this technology. In these years, external field-assisted HER and OER have attracted extensive research interests. Herein, the effects o...
The ionic nature endows halide perovskites with intrinsic interfacial defects in the formed polycrystalline films, thus imposing the challenge of synchronously passivating these defects with low formation energies that directly account for the unsatisfied performance of perovskite solar cells (PSCs). By virtue of the theoretically proven capability of a three to four times enhancement of the formation energy of each defect of Pb‐I antisite (PbI) and iodine vacancy (VI), a new passivation molecule of 1,10‐phenanthrolin‐5‐amine (PAA) is intentionally explored to synchronously passivate the dual defects. The pronounced passivation effect is experimentally verified by the sharp enhancement of the open‐circuit voltage in ternary PSCs from the original 1.118 up to 1.207 V, as well as the construction of PAA‐modified formamidinium lead iodide PSCs with a champion efficiency up to 24.06%, thus providing a universal alternative of addressing interfacial charge carrier dynamics and operational stability of PSCs that are bothered by the multiple interfacial defects.
Tackling the interfacial loss in emerged perovskite‐based solar cells (PSCs) to address synchronously the carrier dynamics and the environmental stability, has been of fundamental and viable importance, while technological hurdles remain in not only creating such interfacial mediator, but the subsequent interfacial embedding in the active layer. This article reports a strategy of interfacial embedding of hydrophobic fluorinated‐gold‐clusters (FGCs) for highly efficient and stable PSCs. The p‐type semiconducting feature enables the FGC efficient interfacial mediator to improve the carrier dynamics by reducing the interfacial carrier transfer barrier and boosting the charge extraction at grain boundaries. The hydrophobic tails of the gold clusters and the hydrogen bonding between fluorine groups and perovskite favor the enhancement of environmental stability. Benefiting from these merits, highly efficient formamidinium lead iodide PSCs (champion efficiency up to 24.02%) with enhanced phase stability under varied relative humidity (RH) from 40% to 95%, as well as highly efficient mixed‐cation PSCs with moisture stability (RH of 75%) over 10 000 h are achieved. It is thus inspiring to advance the development of highly efficient and stable PSCs via interfacial embedding laser‐generated additives for improved charge transfer/extraction and environmental stability.
Superwetting membranes with opposite wettability to oil and water have drawn intense attention in recent years for oil/water separation. Superhydrophilic and underwater superoleophobic membranes have shown unique advantages in the efficient treatment of oily wastewater containing oil-in-water emulsions. Facile interfacial engineering and microstructural design of the hierarchical architectures and the hydrophilic chemistry is of significance but still challenging. In this study, a hydrophilic hierarchical hybrid layer derived from metal−phenolic network (MPN)/metal−organic framework (MOF) synergy is constructed on the membrane surface via a proposed coordination-directed alternating assembly strategy. The assembly of MPN multilayers provides a hydrophilic chemical basis, and the assembly of MOF nanocrystals provides a hierarchical structural basis. Notably, the coordination interfacial interaction enables the formation of well-defined hydrophilic hierarchical architectures. The obtained membrane is thus endowed with robust superhydrophilicity, underwater superoleophobicity, and anti-oil-adhesion capability, which make it capable of highly efficient oil− water separation with high water permeance (above 6300 L/m 2 h), high oil rejection (above 99.4%), and recyclable antifouling property. The high performance of the developed superwetting membrane makes it a competitive candidate for oil/water separation. Additionally, the demonstrated MPN/MOF assembly strategy may offer new prospects for the facile and versatile design of other superwetting materials.
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