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result(s) for
"Cheng, Hefeng"
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A scalable solar-driven photocatalytic system for separated H2 and O2 production from water
by
Wang, Peng
,
Wu, Yaqiang
,
Sakurai, Takuya
in
639/301/299/890
,
639/4077/909/4086
,
639/638/439/890
2025
Solar-driven photocatalytic water splitting offers a sustainable pathway to produce green hydrogen, yet its practical application encounters several challenges including inefficient photocatalysts, sluggish water oxidation, severe reverse reactions and the necessity of separating produced hydrogen and oxygen gases. Herein, we design and develop a photocatalytic system composed of two separate reaction parts: a hydrogen evolution cell containing halide perovskite photocatalysts (MoSe
2
-loaded CH(NH
2
)
2
PbBr
3-x
I
x
) and an oxygen evolution cell containing NiFe-layered double hydroxide modified BiVO
4
photocatalysts. These components are bridged by a I
3
−
/I
−
redox couple to facilitate electron transfer, realizing efficient overall water splitting with a solar-to-hydrogen conversion efficiency of 2.47 ± 0.03%. Additionally, an outdoor scaled-up setup of 692.5 cm
2
achieves an average solar-to-hydrogen conversion efficiency of 1.21% during a week-long test under natural sunlight. By addressing major limitations inherent in conventional photocatalytic systems, such as the cooccurrence of hydrogen and oxygen in a single cell and the resultant severe reverse reactions from hydrogen and oxygen recombination, this work introduces an alternative concept for photocatalytic system design, which enhances both efficiency and practicality.
Photocatalytic water splitting offers a sustainable method for producing green hydrogen but faces challenges due to inefficient materials and systems. Here, the authors report a design for a photocatalytic water-splitting system that efficiently produces hydrogen and oxygen in separate cells.
Journal Article
Selective photoelectrochemical synthesis of adipic acid using single-atom Ir decorated α-Fe2O3 photoanode
2025
Photoelectrochemical (PEC) synthesis offers a sustainable route for fine chemicals production, yet comprehending and modulating the reaction processes at the atomic level remains a challenge. Herein, we develop a single-atom Ir decorated Ti-doped
α
-Fe
2
O
3
photoanode for selective PEC synthesis of adipic acid from cyclohexanone using water as the oxygen source. The PEC system achieves 6.0 μmol cm
–2
h
–1
adipic acid production with ~60% Faradaic efficiency and ~88% selectivity. The single-atom Ir promotes the photogenerated carrier separation and transfer, while regulating the electronic structure of Ti-doped
α
-Fe
2
O
3
photoanode to optimize its adsorption strength of OH
–
and cyclohexanone. Mechanistic studies reveal a non-free-radical reaction pathway at the atomic level, driven by photogenerated holes through an adsorbed hydroxyl transfer. Notably, integrating the photoanode and an amorphous silicon-based photocathode leads to a bias-free PEC device that enables stable adipic acid production for over 80 hours, underscoring the potential for sustainable light-driven synthesis.
The authors report a single-atom Ir-decorated Ti-doped α-Fe
2
O
3
photoanode for bias-free photoelectrochemical adipic acid synthesis via a non-free-radical pathway, achieving high efficiency, selectivity and stability using water as the oxygen source.
Journal Article
Characterization, comparative phylogenetic, and gene transfer analyses of organelle genomes of Rhododendron × pulchrum
2022
Rhododendron × pulchrum , an important horticultural species, is widely distributed in Europe, Asia, and North America. To analyze the phylogenetic and organelle genome information of R. × pulchrum and its related species, the organelle genome of R. × pulchrum was sequenced and assembled. The complete mitochondrial genome showed lineage DNA molecules, which were 816,410 bp long and contained 64 genes, namely 24 transfer RNA (tRNA) genes, 3 ribosomal RNA (rRNA) genes, and 37 protein-coding genes. The chloroplast genome of R. × pulchrum was reassembled and re-annotated; the results were different from those of previous studies. There were 42 and 46 simple sequence repeats (SSR) identified from the mitochondrial and chloroplast genomes of R. × pulchrum , respectively. Five genes ( nad1 , nad2 , nad4 , nad7 , and rps3 ) were potentially useful molecular markers. The R. × pulchrum mitochondrial genome collinear alignment among five species of the Ericaceae showed that the mitochondrial genomes of these related species have a high degree of homology with R. × pulchrum in this gene region, and the most conservative genes were trnC-GCA , trnD-GUC , trnM-CAU , trnN-GUU , trnY-GUA , atp4 , nad4 , nad2 , nad5 , ccmC , and rrn26 . The phylogenetic trees of mitochondrial genome showed that R . simsii was a sister to R. × pulchrum . The results verified that there was gene rearrangement between R. × pulchrum and R . simsii mitochondrial genomes. The codon usage bias of 10 Ericaceae mitochondrial genes and 7 Rhododendron chloroplast genes were influenced by mutation, while other genes codon usages had undergone selection. The study identified 13 homologous fragments containing gene sequences between the chloroplast and mitochondrial genomes of R. × pulchrum . Overall, our results illustrate the organelle genome information could explain the phylogenetics of plants and could be used to develop molecular markers and genetic evolution. Our study will facilitate the study of population genetics and evolution in Rhododendron and other genera in Ericaceae.
Journal Article
Strain Adjustment Realizes the Photocatalytic Overall Water Splitting on Tetragonal Zircon BiVO4
2022
Overall water splitting to generate H2 and O2 is vital in solving energy problem. It is still a great challenge to seek efficient visible light photocatalyst to realize overall water splitting. In this work, the tetragonal zircon BiVO4 is prepared by epitaxial growth on FTO substrate and its overall water splitting reaction is studied. Under the influence of epitaxial strain, the conduction band position shifts negatively and beyond H+/H2 reduction potential (0 V vs NHE), which enables it to possess the photocatalytic hydrogen evolution activity. After loading cocatalysts, the overall water splitting (λ > 400 nm) is realized (H2: ≈65.7 µmol g−1 h−1, O2: ≈32.6 µmol g−1 h−1), and the value of solar hydrogen conversion efficiency is 0.012%. The single‐particle photoluminescence (PL) spectra and PL decay kinetics tests demonstrate the cocatalysts are beneficial to the separation and transfer of carriers. The new strategy of adjusting the band structure by strain is provided. Under the influence of epitaxial strain, the conduction band position of tetragonal zircon BiVO4 grown on FTO substrate can across the H+/H2 reduction potential (0 V vs NHE), achieving overall water splitting under visible light. This work provides a new strategy of adjusting the band structure by strain for performing photocatalytic overall water splitting on BiVO4.
Journal Article
Asymmetric Cu(I)─W Dual‐Atomic Sites Enable C─C Coupling for Selective Photocatalytic CO2 Reduction to C2H4
by
Wang, Peng
,
Mao, Yuyin
,
Song, Kepeng
in
asymmetric dual sites
,
C2H4 generation
,
CO2 photoreduction
2024
Solar‐driven CO2 reduction into value‐added C2+ chemical fuels, such as C2H4, is promising in meeting the carbon‐neutral future, yet the performance is usually hindered by the high energy barrier of the C─C coupling process. Here, an efficient and stabilized Cu(I) single atoms‐modified W18O49 nanowires (Cu1/W18O49) photocatalyst with asymmetric Cu─W dual sites is reported for selective photocatalytic CO2 reduction to C2H4. The interconversion between W(V) and W(VI) in W18O49 ensures the stability of Cu(I) during the photocatalytic process. Under light irradiation, the optimal Cu1/W18O49 (3.6‐Cu1/W18O49) catalyst exhibits concurrent high activity and selectivity toward C2H4 production, reaching a corresponding yield rate of 4.9 µmol g−1 h−1 and selectivity as high as 72.8%, respectively. Combined in situ spectroscopies and computational calculations reveal that Cu(I) single atoms stabilize the *CO intermediate, and the asymmetric Cu─W dual sites effectively reduce the energy barrier for the C─C coupling of two neighboring CO intermediates, enabling the highly selective C2H4 generation from CO2 photoreduction. This work demonstrates leveraging stabilized atomically‐dispersed Cu(I) in asymmetric dual‐sites for selective CO2‐to‐C2H4 conversion and can provide new insight into photocatalytic CO2 reduction to other targeted C2+ products through rational construction of active sites for C─C coupling. An efficient Cu(I) single atoms‐modified W18O49 (Cu1/W18O49) photocatalyst is rationally designed for photocatalytic CO2 reduction to C2H4. Compared to W18O49 that produces CO only, Cu(I) single atoms stabilize *CO intermediates and the asymmetric Cu─W dual sites significantly reduce the energy barrier of C─C coupling, thus leading to the highly selective C2H4 generation from CO2 photoreduction in Cu1/W18O49.
Journal Article
Revealing the Lattice Carbonate Mediated Mechanism in Cu2(OH)2CO3 for Electrocatalytic Reduction of CO2 to C2H4
2024
Understanding the CO2 transformation mechanism on materials is essential for the design of efficient electrocatalysts for CO2 reduction. In aconventional adsorbate evolution mechanism (AEM), the catalysts encounter multiple high‐energy barrier steps, especially CO2 activation, limiting the activity and selectivity. Here, lattice carbonate from Cu2(OH)2CO3 is revealed to be a mediator between CO2 molecules and catalyst during CO2 electroreduction by a 13C isotope labeling method, which can bypass the high energy barrier of CO2 activation and strongly enhance the performance. With the lattice carbonate mediated mechanism (LCMM), the Cu2(OH)2CO3 electrode exhibited ten‐fold faradaic efficiency and 15‐fold current density for ethylene production than the Cu2O electrode with AEM at a low overpotential. Theoretical calculations and in situ Raman spectroscopy results show that symmetric vibration of carbonate is precisely enhanced on the catalyst surface with LCMM, leading to faster electron transfer, and lower energy barriers of CO2 activation and carbon–carbon coupling. This work provides a route to develop efficient electrocatalysts for CO2 reduction based on lattice‐mediated mechanism. Lattice carbonate in Cu2(OH)2CO3 is found to be a mediator linking CO2 molecules with catalyst during CO2 electroreduction by a 13C isotope labeling experiment. Following the lattice carbonate mediated mechanism (LCMM), the Cu2(OH)2CO3 electrode exhibits enhanced ethylene selectivity and activity, which is attributed to the fast electron transfer and reduced energy barriers of CO2 activation and carbon–carbon coupling.
Journal Article
Transcriptome and Flavonoid Compounds Metabolome Analyses Reveal the Mechanisms of Heat Stress in Rhododendron with Exogenously Applied Calcium
2024
Rhododendron plants have ornamental, commercial, and medicinal value to people. Flavonoids are one of the components used in traditional remedies, and Rhododendron plants are found to be rich in flavonoids. Flavonoids can reduce the risk of human disease and participate in the regulation of antioxidant defense systems in response to heat stress. Rhododendron prefers cold climates, so the relatively high temperatures of cities affect the extraction of medicinal ingredients and limit the cultivation environment. Recent studies found that the exogenous application of calcium acts to alleviate heat stress in Rhododendron plants. This study explores the mechanism by which exogenous calcium alleviates heat stress and the role of flavonoids in regulating the antioxidative system in Rhododendron × pulchrum Sweet using combined transcriptomic and metabolomic methods. The activities of peroxidase, catalase and superoxide enzymes were found to increase in response to heat stress and external CaCl2 in the leaves of R. × pulchrum. In total, 433 metabolic components and 370 DEGs were identified as being differentially expressed in response to heat stress and external calcium chloride (CaCl2) in the leaves of R. × pulchrum. These results illustrate that heat stress induces oxidative stress and that external CaCl2 can enhance the heat tolerance of Rhododendron. Flavonoid compounds are responsible for the antioxidant scavenging of reactive oxygen species in R. × pulchrum leaves exposed to heat stress and external calcium.
Journal Article
Reinforcing the Efficiency of Plastic Upgrading through Full‐Spectrum Photothermal Effect Integration of Heat Isolator
by
Wang, Peng
,
Lv, Min
,
Gong, Xueqin
in
alkali‐free hydrothermal pretreatment
,
Catalysis
,
Efficiency
2024
Photoreforming of polyethylene terephthalate (PET) to H2 is practically attractive strategy for upgrading waste plastics. The major challenge is to utilize the infrared energy in the solar spectrum to improve the efficiency for photoreforming of PET to H2. Herein, through the ingenious integration of tungsten phosphide nanoparticles and tungsten single atoms (WP/W SAs) with carbon nitride (g‐C3N4), the constructed hybrid inherits both the desirable properties and structural merits of the respective building blocks. Specifically, the photothermal effect of WP/W SAs couples with the “heat isolator” role of g‐C3N4 due to its low thermal conductivity, thereby forming localized high‐temperature regions, reducing the activation energy and improving the kinetics in the photoreforming of PET to H2. Additionally, the green pretreatment of PET using alkali‐free hydrothermal strategy is reported, achieving direct separation of the ethylene glycol and terephthalic acid. This work not only provides an alkali‐free hydrothermal pretreatment for PET, but also integrates the photothermal effect with the thermal insulation and opens a new avenue for harnessing solar energy into to convert plastics into H2. To enhance the activity for photoreforming of PET to H2, the photothermal effect of WP/W SAs couples with the “heat isolator” role of g‐C3N4 due to its low thermal conductivity, thereby forming localized high‐temperature regions and reducing the activation energy. Additionally, a strategy of alkali‐free hydrothermal pretreatment of PET is reported, achieving direct separation of ethylene glycol and terephthalic acid.
Journal Article
Comprehensive Genomic Survey, Structural Classification, and Expression Analysis of WRKY Transcription Factor Family in Rhododendron simsii
2022
(1) Rhododendron is one of the top ten traditional flowers in China, with both high ornamental and economic values. However, with the change of the environment, Rhododendron suffers from various biological stresses. The WRKY transcription factor is a member of the most crucial transcription factor families, which plays an essential regulatory role in a variety of physiological processes and developmental stresses. (2) In this study, 57 RsWRKYs were identified using genome data and found to be randomly distributed on 13 chromosomes. Based on gene structure and phylogenetic relationships, 57 proteins were divided into three groups: I, II, and III. Multiple alignments of RsWRKYs with Arabidopsis thaliana homologous genes revealed that WRKY domains in different groups had different conserved sites. RsWRKYs have a highly conserved domain, WRKYGQK, with three variants, WRKYGKK, WRKYGEK, and WRKYGRK. Furthermore, cis-acting elements analysis revealed that all of the RsWRKYs had stress and plant hormone cis-elements, with figures varying by group. Finally, the expression patterns of nine WRKY genes treated with gibberellin acid (GA), methyl jasmonate (MeJA), heat, and drought in Rhododendron were also measured using quantitative real-time PCR (qRT-PCR). The results showed that the expression levels of the majority of RsWRKY genes changed in response to multiple phytohormones and abiotic stressors. (3) This current study establishes a theoretical basis for future studies on the response of RsWRKY transcription factors to various hormone and abiotic stresses as well as a significant foundation for the breeding of new stress-tolerant Rhododendron varieties.
Journal Article
Beneficial Effect of Exogenously Applied Calcium Chloride on the Anatomy and Fast Chlorophyll Fluorescence in Rhododendron × pulchrum Leaves Following Short-Term Heat Stress Treatment
2022
The heat tolerance of plants can be improved by using exogenous calcium chloride (CaCl2) to cope with temperature fluctuations. Since global climates continue to warm, it is important to further explore the way in which plants respond to heat stress with the use of CaCl2. We aimed to explore the effect of exogenous CaCl2 on the leaf microstructure, leaf epidermal ultrastructure, and chlorophyll a fluorescence of Rhododendron × pulchrum (R. × pulchrum) under heat stress. In the leaves of R. × pulchrum treated with exogenous CaCl2, compared to the control, the thickness of the epidermis, spongy tissues, and stomatal aperture increased, whereas the stomata density and ratio of closed/open stomata decreased. In the leaves of R. × pulchrum under heat stress conditions, compared to the control, the values of the maximal photochemical efficiency of photosystem II (Fv/Fm), the performance index on an absorption basis (PIABS), the quantum yield for the reduction of terminal electron acceptors on the acceptor side of PSI (φRo), and the energy absorbed per unit cross-section of a photosynthesizing object at the moment of achieving the fluorescence maximum (ABS/CSM) all decreased, whereas the quantum yield of the energy dissipation (φDo) increased significantly. However, these differences disappeared when R. × pulchrum was treated with exogenous CaCl2. This suggests that exogenous CaCl2 can improve the heat tolerance in R. × pulchrum by regulating the leaf anatomical structure and the behavior of epidermal cells and stomata in leaves, protecting the stability of photosystems I and II and improving the electron transfer from QA to QB. Our study could provide a theoretical basis for the breeding, further research, and utilization of Rhododendron in the context of global warming.
Journal Article