Electrocatalytic carbon dioxide reduction to formate is desirable but challenging. Current attention is mostly focused on tin-based materials, which, unfortunately, often suffer from limited Faradaic efficiency. The potential of bismuth in carbon dioxide reduction has been suggested but remained understudied. Here, we report that ultrathin bismuth nanosheets are prepared from the in situ topotactic transformation of bismuth oxyiodide nanosheets. They process single crystallinity and enlarged surface areas. Such an advantageous nanostructure affords the material with excellent electrocatalytic performance for carbon dioxide reduction to formate. High selectivity (~100%) and large current density are measured over a broad potential, as well as excellent durability for >10 h. Its selectivity for formate is also understood by density functional theory calculations. In addition, bismuth nanosheets were coupled with an iridium-based oxygen evolution electrocatalyst to achieve efficient full-cell electrolysis. When powered by two AA-size alkaline batteries, the full cell exhibits impressive Faradaic efficiency and electricity-to-formate conversion efficiency.
Formic acid (or formate) is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction. However, its commercial viability hinges on the development of highly active and selective electrocatalysts. Here we report that structural defects have a profound positive impact on the electrocatalytic performance of bismuth. Bismuth oxide double-walled nanotubes with fragmented surface are prepared as a template, and are cathodically converted to defective bismuth nanotubes. This converted electrocatalyst enables carbon dioxide reduction to formate with excellent activity, selectivity and stability. Most significantly, its current density reaches ~288 mA cm
−2
at −0.61 V versus reversible hydrogen electrode within a flow cell reactor under ambient conditions. Using density functional theory calculations, the excellent activity and selectivity are rationalized as the outcome of abundant defective bismuth sites that stabilize the *OCHO intermediate. Furthermore, this electrocatalyst is coupled with silicon photocathodes and achieves high-performance photoelectrochemical carbon dioxide reduction.
The development of highly active and stable electrocatalysts for ethanol electroxidation is of decisive importance to the successful commercialization of direct ethanol fuel cells. Despite great efforts invested over the past decade, their progress has been notably slower than expected. In this work, the facile solution synthesis of 2D PdAg alloy nanodendrites as a high-performance electrocatalyst is reported for ethanol electroxidation. The reaction is carried out via the coreduction of Pd and Ag precursors in aqueous solution with the presence of octadecyltrimethylammonium chloride as the structural directing agent. Final products feature small thickness (5-7 nm) and random in-plane branching with enlarged surface areas and abundant undercoordinated sites. They exhibit enhanced electrocatalytic activity (large specific current ≈2600 mA mgPd-1) and excellent operation stability (as revealed from both the cycling and chronoamperometric tests) for ethanol electroxidation. Control experiments show that the improvement comes from the combined electronic and structural effects.
The conversion of CO 2 to value-added products using electrical or solar energy represents an attractive means for the capture and utilization of atmospheric CO 2 . Formate is a popular product from CO 2 reduction, but its reaction selectivity is usually unsatisfactory. Tin-based materials have attracted most attention for formate production at present. Unfortunately, most of them only exhibit moderate selectivity in a narrow and highly cathodic potential window. In this study, we demonstrate that traditionally under-explored bismuth has a much greater potential for formate production than tin or other materials. Mesoporous bismuth nanosheets are prepared here by the cathodic transformation of atomic-thick bismuth oxycarbonate nanosheets. They enable the selective CO 2 reduction to formate with large current density, excellent Faradaic efficiency (~100%) over a broad potential window and great operation stability. Moreover, we integrate Bi nanosheets with an oxygen evolution reaction electrocatalyst in full cells, and achieve efficient and robust solar conversion of CO 2 /H 2 O to formate/O 2 .
Based on the properties comparison between FDCA-based epoxy and TPA-based epoxy, FDCA has been regarded as an ideal renewable platform chemical for the synthesis of thermosetting resins with high performance.
Many problems associated with Li-S and Na-S batteries essentially root in the generation of their soluble polysulfide intermediates. While conventional wisdom mainly focuses on trapping polysulfides at the cathode using various functional materials, few strategies are available at present to fully resolve or circumvent this long-standing issue. In this study, we propose the concept of sulfur-equivalent cathode materials, and demonstrate the great potential of amorphous MoS as such a material for room-temperature Li-S and Na-S batteries. In Li-S batteries, MoS exhibits sulfur-like behavior with large reversible specific capacity, excellent cycle life, and the possibility to achieve high areal capacity. Most remarkably, it is also fully cyclable in the carbonate electrolyte under a relatively high temperature of 55 °C. MoS can also be used as the cathode material of even more challenging Na-S batteries to enable decent capacity and good cycle life. X-ray absorption spectroscopy (XAS) experiments are carried out to track the structural evolution of MoS It largely preserves its chain-like structure during repetitive battery cycling without generating any free polysulfide intermediates.
Surface passivation is an effective approach to eliminate defects and thus to achieve efficient perovskite solar cells, while the stability of the passivation effect is a new concern for device stability engineering. Herein, tribenzylphosphine oxide (TBPO) is introduced to stably passivate the perovskite surface. A high efficiency exceeding 22%, with steady‐state efficiency of 21.6%, is achieved, which is among the highest performances for TiO2 planar cells, and the hysteresis is significantly suppressed. Further density functional theory (DFT) calculation reveals that the surface molecule superstructure induced by TBPO intermolecular π–π conjugation, such as the periodic interconnected structure, results in a high stability of TBPO–perovskite coordination and passivation. The passivated cell exhibits significantly improved stability, with sustaining 92% of initial efficiency after 250 h maximum‐power‐point tracking. Therefore, the construction of a stabilized surface passivation in this work represents great progress in the stability engineering of perovskite solar cells.
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