Electrocatalytic conversion of nitrogen oxides to value-added chemicals is a promising strategy for mitigating the human-caused unbalance of the global nitrogen-cycle, but controlling product selectivity remains a great challenge. Here we show iron–nitrogen-doped carbon as an efficient and durable electrocatalyst for selective nitric oxide reduction into hydroxylamine. Using in operando spectroscopic techniques, the catalytic site is identified as isolated ferrous moieties, at which the rate for hydroxylamine production increases in a super-Nernstian way upon pH decrease. Computational multiscale modelling attributes the origin of unconventional pH dependence to the redox active (non-innocent) property of NO. This makes the rate-limiting NO adsorbate state more sensitive to surface charge which varies with the pH-dependent overpotential. Guided by these fundamental insights, we achieve a Faradaic efficiency of 71% and an unprecedented production rate of 215 μmol cm−2 h−1 at a short-circuit mode in a flow-type fuel cell without significant catalytic deactivation over 50 h operation.
'Ideal' transparent p-type semiconductors are required for the integration of high-performance thin-film transistors (TFTs) and circuits. Although CuI has recently attracted attention owing to its excellent opto-electrical properties, solution processability, and low-temperature synthesis, the uncontrolled copper vacancy generation and subsequent excessive hole doping hinder its use as a semiconductor material in TFT devices. In this study, we propose a doping approach through soft chemical solution process and transparent p-type Zn-doped CuI semiconductor for high-performance TFTs and circuits. The optimised TFTs annealed at 80°C exhibit a high hole mobility of over 5 cm 2 V −1 s −1 and high on/off current ratio of~10 7 with good operational stability and reproducibility. The CuI:Zn semiconductors show intrinsic advantages for next-generation TFT applications and wider applications in optoelectronics and energy conversion/storage devices. This study paves the way for the realisation of transparent, flexible, and large-area integrated circuits combined with n-type metal-oxide semiconductor.
Chemical barriers contribute to nonhost resistance, which is defined as the resistance of an entire plant species to nonadapted pathogen species. However, the molecular basis of metabolic defense in nonhost resistance remains elusive. Here, we report genetic evidence for the essential role of phytoalexin capsidiol in nonhost resistance of pepper (Capsicum spp.) to potato late blight Phytophthora infestans using transcriptome and genome analyses. Two different genes for capsidiol biosynthesis, 5-epi-aristolochene synthase (EAS) and 5-epi-aristolochene-1,3-dihydroxylase (EAH), belong to multigene families. However, only a subset of EAS/EAH gene family members were highly induced upon P. infestans infection, which was associated with parallel accumulation of capsidiol in P. infestans-infected pepper. Silencing of EAS homologs in pepper resulted in a significant decrease in capsidiol accumulation and allowed the growth of nonadapted P. infestans that is highly sensitive to capsidiol. Phylogenetic and genomic analyses of EAS/EAH multigene families revealed that the emergence of pathogen-inducible EAS/EAH genes in Capsicum-specific genomic regions rendered pepper a nonhost of P. infestans. This study provides insights into evolutionary aspects of nonhost resistance based on the combination of a species-specific phytoalexin and sensitivity of nonadapted pathogens.
Although n-type transparent conductors have been commercialized
with high optical transmittance and electrical conductivity, the realization
of their p-type counterparts has been a challenging problem. Here,
we report the synthesis of a highly conductive transparent p-type
sulfur-doped CuI (CuI:S) thin film using a liquid-iodination method
with a thiol additive. The CuI:S film shows a remarkably high electrical
conductivity of 511 S cm–1 with an optical transmittance
of greater than 80%. Furthermore, additional hole doping of CuI:S
with H2O2 treatment improves the electrical
conductivity to 596 S cm–1. Consequently, CuI:S
exhibits a record-high figure of merit (FOM) value of 63,000 M Ω–1 (73,000 M Ω–1 with H2O2 treatment), which is ∼370% (∼430%
with H2O2 treatment) higher than the previously
reported record-high FOM value. The highly conducting CuI:S electrode
is successfully applied as transparent conducting electrodes of the
organic light-emitting diode and transparent p-type thin-film transistor.
The liquid-iodination chemical method with unconventional control
of the reaction parameters can be generalized to produce high-quality
metal halide thin films, allowing them to be applicable for transparent
electronics and optoelectronics.
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