Electrocatalytic N reduction reaction (NRR) to synthesize ammonia is a sustainable reaction that is expected to replace Haber Bosch process. Laminated BiWO has great potential as an NRR electrocatalyst, however, the effective activity requires that the inert substrate is fully activated. Here, for the first time, success is achieved in activating the BiWO basal planes with NRR activity through Ti doping.
View Article and Find Full Text PDFNitrate and nitrite (NO) are widespread contaminants in industrial wastewater and groundwater. Sustainable ammonia (NH) production via NO electroreduction provides a prospective alternative to the energy-intensive industrialized Haber-Bosch process. However, selectively regulating the reaction pathway, which involves complicated electron/proton transfer, toward NH generation relies on the robust catalyst.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2020
Closing the anthropogenic carbon cycle by converting CO into reusable chemicals is an attractive solution to mitigate rising concentrations of CO in the atmosphere. Herein, we prepared Ni metal catalysts ranging in size from single atoms to over 100 nm and distributed them across N-doped carbon substrates which were obtained from converted zeolitic imidazolate frameworks (ZIF). The results show variance in CO reduction performance with variance in Ni metal size.
View Article and Find Full Text PDFWater and energy systems are interdependent: water is utilized in each stage of energy production, and energy is required to extract, treat, and deliver water for many uses. However, energy and water systems are usually developed and managed independently. In the quest to develop environmentally friendly and energy-efficient solutions for water and energy issues, photoelectrochemical (PEC) energy conversion and microbial electrochemical (MEC) systems show profound potential for addressing environmental remediation problems and harvesting energy simultaneously.
View Article and Find Full Text PDFDespite the fact that many strategies have been developed to improve the efficiency of the oxygen evolution reaction (OER), the precise modulation of the surface electronic properties of catalysts to improve their catalytic activity is still challenging. Herein, we demonstrate that the surface active electron density of Co O can be effectively regulated by an argon-ion irradiation method. X-ray photoelectron and synchrotron x-ray absorption spectroscopy, UV photoelectron spectrometry, and DFT calculations show that the surface active electron density band center of Co O has been upshifted, leading to a significantly enhanced absorption capability of the oxo group.
View Article and Find Full Text PDFAn N-doped TiO model reveals a conceptually different mechanism for activating the N dopant based on delocalized orbital hybridization through O vacancy incorporation. Synchrotron-based X-ray absorption spectroscopy, time-resolved fluorescence, and DFT studies revealed that O vacancy incorporation can effectively stimulate the delocalization of N impurity states through p-band orbital modulation, which leads to a significant enhancement in photocarrier lifetime. Consequently, this effect also results in a remarkable increase in the incident photon-to-electron conversion efficiency in the range of 400-550 nm compared to that of conventional N-incorporated TiO (15 % versus 1 % at 450 nm).
View Article and Find Full Text PDFExploring highly active, enduringly stable, and low-cost oxygen evolution reaction catalysts continues to be a dominant challenge to commercialize renewable electrochemical water-splitting technology. High-active and earth-abundant cobalt phosphides are recently considered as promising candidates. However, the poor inherent electron transfer efficiency and instability hinder its further development.
View Article and Find Full Text PDFThe metal-oxide semiconductor TiO shows enormous potential in the field of photoelectric detection; however, UV-light absorption only restricts its widespread application. It is considered that nitrogen doping can improve the visible light absorption of TiO, but the effect of traditional chemical doping is far from being used for visible light detection. Herein, we dramatically broadened the absorption spectrum of the TiO nanowire (NW) by nitrogen ion implantation and apply the N-doped single TiO NW to visible light detection for the first time.
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