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1.
ACS Appl Mater Interfaces ; 16(19): 25246-25255, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38696547

ABSTRACT

Ion transportation via the mixed mechanisms of hydrogels underpins ultrafast biological signal transmission in nature, and its application to the rapid and sensitive sensing detection of human specific ions is of great interest for the field of medical science. However, current research efforts are still unable to achieve transmission results that are comparable to those of bioelectric signals. Herein, 3D interconnected nanochannels based on poly(pyrrole-co-dopamine)/poly(vinyl alcohol) (P(Py-co-DA)/PVA) supernetwork conductive hydrogels are designed and fabricated as stimuli-responsive structures for K+ ions. Distinct from conventional configurations, which exhibit rapid electron transfer and permeability to biosubstrates, interconnected nanofluidic nanochannels collaborated with the P(Py-co-DA) conductive polymer in the supernetwork conductive hydrogel significantly improve conductivity (88.3 mS/cm), ion transport time (0.1 s), and ion sensitivity (74.6 mV/dec). The faster ion response time is attributed to the synergism of excellent conductivity originating from the P(Py-co-DA) polymer and the electronic effect in the interconnected nanofluidic channels. Furthermore, the supernetwork conductive hydrogel demonstrates K+ ion selectivity relative to other cations in biofluids such as Na+, Mg2+, and Ca2+. The DFT calculation indicates that the small solvation energy and low chemical transfer resistance are the main reasons for the excellent K+ ion selectivity. Finite element analysis (FEA) simulations further support these experimental results. Consequently, the P(Py-co-DA)/PVA supernetwork conductive hydrogels enriched with the 3D interconnected nanofluidic channels developed in this work possess excellent sensing of K+ ions. This strategy provides great insight into efficient ion sensing in traditional biomedical sensing that has not been explored by previous researchers.

2.
Dev Cell ; 59(7): 924-939.e6, 2024 Apr 08.
Article in English | MEDLINE | ID: mdl-38359831

ABSTRACT

Brassinosteroid (BR) signaling leads to the nuclear accumulation of the BRASSINAZOLE-RESISTANT 1 (BZR1) transcription factor, which plays dual roles in activating or repressing the expression of thousands of genes. BZR1 represses gene expression by recruiting histone deacetylases, but how it activates transcription of BR-induced genes remains unclear. Here, we show that BR reshapes the genome-wide chromatin accessibility landscape, increasing the accessibility of BR-induced genes and reducing the accessibility of BR-repressed genes in Arabidopsis. BZR1 physically interacts with the BRAHMA-associated SWI/SNF (BAS)-chromatin-remodeling complex on the genome and selectively recruits the BAS complex to BR-activated genes. Depletion of BAS abrogates the capacities of BZR1 to increase chromatin accessibility, activate gene expression, and promote cell elongation without affecting BZR1's ability to reduce chromatin accessibility and expression of BR-repressed genes. Together, these data identify that BZR1 recruits the BAS complex to open chromatin and to mediate BR-induced transcriptional activation of growth-promoting genes.


Subject(s)
Arabidopsis Proteins , Arabidopsis , Arabidopsis/metabolism , Brassinosteroids/metabolism , Chromatin/genetics , Chromatin/metabolism , Arabidopsis Proteins/genetics , Arabidopsis Proteins/metabolism , DNA-Binding Proteins/genetics , DNA-Binding Proteins/metabolism , Transcriptional Activation , Nuclear Proteins/genetics , Nuclear Proteins/metabolism , Gene Expression Regulation, Plant
3.
Nat Commun ; 15(1): 935, 2024 Jan 31.
Article in English | MEDLINE | ID: mdl-38296999

ABSTRACT

Switch defective/sucrose non-fermentable (SWI/SNF) chromatin remodeling complexes are multi-subunit machineries that establish and maintain chromatin accessibility and gene expression by regulating chromatin structure. However, how the remodeling activities of SWI/SNF complexes are regulated in eukaryotes remains elusive. B-cell lymphoma/leukemia protein 7 A/B/C (BCL7A/B/C) have been reported as subunits of SWI/SNF complexes for decades in animals and recently in plants; however, the role of BCL7 subunits in SWI/SNF function remains undefined. Here, we identify a unique role for plant BCL7A and BCL7B homologous subunits in potentiating the genome-wide chromatin remodeling activities of SWI/SNF complexes in plants. BCL7A/B require the catalytic ATPase BRAHMA (BRM) to assemble with the signature subunits of the BRM-Associated SWI/SNF complexes (BAS) and for genomic binding at a subset of target genes. Loss of BCL7A and BCL7B diminishes BAS-mediated genome-wide chromatin accessibility without changing the stability and genomic targeting of the BAS complex, highlighting the specialized role of BCL7A/B in regulating remodeling activity. We further show that BCL7A/B fine-tune the remodeling activity of BAS complexes to generate accessible chromatin at the juvenility resetting region (JRR) of the microRNAs MIR156A/C for plant juvenile identity maintenance. In summary, our work uncovers the function of previously elusive SWI/SNF subunits in multicellular eukaryotes and provides insights into the mechanisms whereby plants memorize the juvenile identity through SWI/SNF-mediated control of chromatin accessibility.


Subject(s)
Chromatin , Transcription Factors , Animals , Chromatin/genetics , Transcription Factors/metabolism , Adenosine Triphosphatases/genetics , Adenosine Triphosphatases/metabolism , Chromatin Assembly and Disassembly , Gene Expression
4.
Small ; 20(10): e2306344, 2024 Mar.
Article in English | MEDLINE | ID: mdl-37875719

ABSTRACT

The coupling of photocatalytic hydrogen production and selective oxidation of benzylamine is a topic of significant research interest. However, enhancing the bifunctional photocatalytic activity in this context is still a major challenge. The construction of Z-scheme heterojunctions is an effective strategy to enhance the activity of bifunctional photocatalysts. Herein, a p-n type direct Z-scheme heterojunction CuS/TiO2 is constructed using metal-organic framework (MOF)-derived TiO2 as a substrate. The carrier density is measured by Mott-Schottky under photoexcitation, which confirms that the Z-scheme electron transfer mode of CuS/TiO2 is driven by the diffusion effect caused by the carrier concentration difference. Benefiting from efficient charge separation and transfer, photogenerated electrons, and holes are directedly transferred to active oxidation and reduction sites. CuS/TiO2 also exhibits excellent bifunctional photocatalytic activity without noble metal cocatalysts. Among them, the H2 evolution activity of the CuS/TiO2 is found to be 17.1 and 29.5 times higher than that of TiO2 and CuS, respectively. Additionally, the yields of N-Benzylidenebenzylamine (NBB) are 14.3 and 47.4 times higher than those of TiO2 and CuS, respectively.

5.
Planta ; 259(1): 8, 2023 Nov 29.
Article in English | MEDLINE | ID: mdl-38019301

ABSTRACT

MAIN CONCLUSION: This study reveals that mutations in BRIP1/2 subunits of the BAS complex disrupt root meristem development by decreasing PIN genes expression, affecting auxin transport, and downregulating essential root genes PLT. Switch defective/sucrose non-fermentable (SWI/SNF) chromatin remodeling complexes play vital roles in plant development. BRAHMA-interacting proteins1 (BRIP1) and BRIP2 are subunits of BRAHMA (BRM)-associated SWI/SNF complex (BAS) in plants; however, their role and underlying regulatory mechanism in root development are still unknown. Here, we show that brip1 brip2 double mutants have a significantly shortened root meristem and an irregular arrangement in a portion of the root stem cell niche. The mutations in BRIP1 and BRIP2 cause decreased expression of the PIN-FORMED (PIN) genes, which in turn reduces the transport of auxin at the root tip, leading to the disruption of the accurate establishment of normal auxin concentration gradients in the stem cells. Chromatin immunoprecipitation (ChIP) experiments indicated that BRIP1 and BRIP2 directly bind to the PINs. Furthermore, we found a significant down-regulation in the expression of key root development genes, PLETHORA (PLT), in brip1 brip2. The brip1 brip2 plt1 plt2 quadruple mutations do not show further exacerbation in the short-root phenotype compared to plt1 plt2 double mutants. Using a dexamethasone (DEX)-inducible PLT2 transgenic line, we showed that acute overexpression of PLT2 partially rescues root meristem defects of brip1 brip2, suggesting that BRIP1 and BRIP2 act in part through the PLT1/2 pathway. Taken together, our results identify the critical role and the underlying mechanism of BRIP1/2 in maintaining the development of root meristem through the regulation of auxin output and expression of PLTs.


Subject(s)
Indoleacetic Acids , Meristem , Plant Proteins , Biological Transport , Down-Regulation , Gene Expression , Meristem/genetics , Plant Proteins/genetics
6.
J Phys Chem Lett ; 14(29): 6532-6541, 2023 Jul 27.
Article in English | MEDLINE | ID: mdl-37450690

ABSTRACT

Organic solar cells (OSCs) have attracted lots of attention owing to their low cost, lightweight, and flexibility properties. Nowadays, the performance of OSCs is continuously improving with the development of active layer materials. However, the traditional hole transport layer (HTL) material Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) presents insufficient conductivity and rapid degradation, which decreases the efficiency and stability of OSCs. To conquer the challenge, the two-dimensional (2D) graphitic carbon nitride (g-C3N4) nanomaterials incorporated into the PEDOT:PSS as hybrid HTL are reported. The addition of g-C3N4 into PEDOT:PSS enables the thickness of the HTL to decrease for enhancing the transmittance of the film and increase the conductivity of PEDOT:PSS. Thus, the device exhibts improved charge transport and suppressed carrier recombination, leading to the increase in short-circuit current density and power conversion efficiency of the devices. This work demonstrates that the incorporation of 2D g-C3N4 into PEDOT:PSS for D18:Y6 and PM6:L8-BO-based OSCs can significantly improve the device efficiency to 17.48% and 18.47% with the enhancement of 7.04% and 8.46%, respectively.

7.
Plant Cell ; 35(7): 2464-2483, 2023 06 26.
Article in English | MEDLINE | ID: mdl-37062961

ABSTRACT

Switch defective/sucrose nonfermentable (SWI/SNF) complexes are evolutionarily conserved multisubunit machines that play vital roles in chromatin architecture regulation for modulating gene expression via sliding or ejection of nucleosomes in eukaryotes. In plants, perturbations of SWI/SNF subunits often result in severe developmental disorders. However, the subunit composition, pathways of assembly, and genomic targeting of the plant SWI/SNF complexes are poorly understood. Here, we report the organization, genomic targeting, and assembly of 3 distinct SWI/SNF complexes in Arabidopsis thaliana: BRAHMA-Associated SWI/SNF complexes (BAS), SPLAYED-Associated SWI/SNF complexes (SAS), and MINUSCULE-Associated SWI/SNF complexes (MAS). We show that BAS complexes are equivalent to human ncBAF, whereas SAS and MAS complexes evolve in multiple subunits unique to plants, suggesting plant-specific functional evolution of SWI/SNF complexes. We further show overlapping and specific genomic targeting of the 3 plant SWI/SNF complexes on chromatin and reveal that SAS complexes are necessary for the correct genomic localization of the BAS complexes. Finally, we define the role of the core module subunit in the assembly of plant SWI/SNF complexes and highlight that ATPase module subunit is required for global complex stability and the interaction of core module subunits in Arabidopsis SAS and BAS complexes. Together, our work highlights the divergence of SWI/SNF chromatin remodelers during eukaryote evolution and provides a comprehensive landscape for understanding plant SWI/SNF complex organization, assembly, genomic targeting, and function.


Subject(s)
Arabidopsis , Humans , Arabidopsis/genetics , Arabidopsis/metabolism , Transcription Factors/genetics , Transcription Factors/metabolism , Chromatin Assembly and Disassembly/genetics , Chromosomal Proteins, Non-Histone/genetics , Chromosomal Proteins, Non-Histone/metabolism , Chromatin/genetics , Chromatin/metabolism , Genomics
8.
Small ; 18(46): e2200510, 2022 Nov.
Article in English | MEDLINE | ID: mdl-36209383

ABSTRACT

To improve the photoelectrochemical (PEC) performance of photocatalysts, the doping strategy through covalent functionalization is often adopted to adjust material electronic structures. By contrast, this work demonstrates that the noncovalent interaction in the case of iodinated graphitic carbon nitride (g-CN) film can also enhance the PEC performance. Through a facile synthesis method of rapid thermal vapor condensation (RTVC), the prepared iodinated g-CN film shows a significantly improved photocurrent density (38.9 µA cm-2 ), three times that of pure g-CN film (13.0 µA cm-2 ) at 1.23 V versus reversible hydrogen electrode. Computations reveal that the noncovalent attachment of iodine anion (I- ) on g-CN plays a crucial role in modulating the bandgap states and broadening of the visible-light absorption range as well as the charge carrier separation with the photo-induced hole confined to I- and electron to g-CN film. The fully filled valence orbitals (4d10 5s2 5p6 ) of I- determine its noncovalent attachment on the g-CN film and so do the iodine species of I3 - , I5 - , etc. This work offers a favorable synthesis method to achieve efficient doping through noncovalent charge transfer between thin film and certain dopants and provides a useful modification strategy for the establishment of multi-channel transportation of charge carriers in general photocatalysts.

9.
Plant Cell ; 34(10): 3915-3935, 2022 09 27.
Article in English | MEDLINE | ID: mdl-35866997

ABSTRACT

PICKLE (PKL) is a chromodomain helicase DNA-binding domain 3 (CHD3) chromatin remodeler that plays essential roles in controlling the gene expression patterns that determine developmental identity in plants, but the molecular mechanisms through which PKL is recruited to its target genes remain elusive. Here, we define a cis-motif and trans-acting factors mechanism that governs the genomic occupancy profile of PKL in Arabidopsis thaliana. We show that two homologous trans-factors VIVIPAROUS1/ABI3-LIKE1 (VAL1) and VAL2 physically interact with PKL in vivo, localize extensively to PKL-occupied regions in the genome, and promote efficient PKL recruitment at thousands of target genes, including those involved in seed maturation. Transcriptome analysis and genetic interaction studies reveal a close cooperation of VAL1/VAL2 and PKL in regulating gene expression and developmental fate. We demonstrate that this recruitment operates at two master regulatory genes, ABSCISIC ACID INSENSITIVE3 and AGAMOUS-LIKE 15, to repress the seed maturation program and ensure the seed-to-seedling transition. Together, our work unveils a general rule through which the CHD3 chromatin remodeler PKL binds to its target chromatin in plants.


Subject(s)
Arabidopsis Proteins , Arabidopsis , Abscisic Acid/metabolism , Arabidopsis/genetics , Arabidopsis/metabolism , Arabidopsis Proteins/genetics , Arabidopsis Proteins/metabolism , Chromatin/genetics , Chromatin/metabolism , DNA/metabolism , DNA Helicases/genetics , DNA Helicases/metabolism , Gene Expression Regulation, Plant/genetics , Seeds/genetics , Trans-Activators/metabolism , Transcription Factors/genetics , Transcription Factors/metabolism
10.
Mol Plant ; 14(6): 888-904, 2021 06 07.
Article in English | MEDLINE | ID: mdl-33771698

ABSTRACT

Switch defective/sucrose non-fermentable (SWI/SNF) chromatin remodeling complexes are multi-subunit machines that play vital roles in the regulation of chromatin structure and gene expression. However, the mechanisms by which SWI/SNF complexes recognize their target loci in plants are not fully understood. Here, we show that the Arabidopsis thaliana bromodomain-containing proteins BRD1, BRD2, and BRD13 are core subunits of SWI/SNF complexes and critical for SWI/SNF genomic targeting. These three BRDs interact directly with multiple SWI/SNF subunits, including the BRAHMA (BRM) catalytic subunit. Phenotypic and transcriptomic analyses of the brd1 brd2 brd13 triple mutant revealed that these BRDs act largely redundantly to control gene expression and developmental processes that are also regulated by BRM. Genome-wide occupancy profiling demonstrated that these three BRDs extensively colocalize with BRM on chromatin. Simultaneous loss of function of three BRD genes results in reduced BRM protein levels and decreased occupancy of BRM on chromatin across the genome. Furthermore, we demonstrated that the bromodomains of BRDs are essential for genomic targeting of the BRD subunits of SWI/SNF complexes to their target sites. Collectively, these results demonstrate that BRD1, BRD2, and BRD13 are core subunits of SWI/SNF complexes and reveal their biological roles in facilitating genomic targeting of BRM-containing SWI/SNF complexes in plants.


Subject(s)
Adenosine Triphosphatases/metabolism , Arabidopsis Proteins/metabolism , Arabidopsis/metabolism , Chromatin Assembly and Disassembly , Chromosomal Proteins, Non-Histone/metabolism , Transcription Factors/metabolism , Adenosine Triphosphatases/genetics , Arabidopsis/genetics , Arabidopsis/growth & development , Arabidopsis Proteins/genetics , Chromatin/metabolism , Chromosomal Proteins, Non-Histone/chemistry , Gene Expression Profiling , Gene Expression Regulation, Plant , Transcription Factors/chemistry
11.
Plant Physiol ; 186(1): 534-548, 2021 05 27.
Article in English | MEDLINE | ID: mdl-33620498

ABSTRACT

In flowering plants, repression of the seed maturation program is essential for the transition from the seed to the vegetative phase, but the underlying mechanisms remain poorly understood. The B3-domain protein VIVIPAROUS1/ABSCISIC ACID-INSENSITIVE3-LIKE 1 (VAL1) is involved in repressing the seed maturation program. Here we uncovered a molecular network triggered by the plant hormone brassinosteroid (BR) that inhibits the seed maturation program during the seed-to-seedling transition in Arabidopsis (Arabidopsis thaliana). val1-2 mutant seedlings treated with a BR biosynthesis inhibitor form embryonic structures, whereas BR signaling gain-of-function mutations rescue the embryonic structure trait. Furthermore, the BR-activated transcription factors BRI1-EMS-SUPPRESSOR 1 and BRASSINAZOLE-RESISTANT 1 bind directly to the promoter of AGAMOUS-LIKE15 (AGL15), which encodes a transcription factor involved in activating the seed maturation program, and suppress its expression. Genetic analysis indicated that BR signaling is epistatic to AGL15 and represses the seed maturation program by downregulating AGL15. Finally, we showed that the BR-mediated pathway functions synergistically with the VAL1/2-mediated pathway to ensure the full repression of the seed maturation program. Together, our work uncovered a mechanism underlying the suppression of the seed maturation program, shedding light on how BR promotes seedling growth.


Subject(s)
Arabidopsis Proteins/genetics , Arabidopsis/growth & development , Brassinosteroids/metabolism , MADS Domain Proteins/genetics , Repressor Proteins/genetics , Seedlings/growth & development , Seeds/growth & development , Arabidopsis/genetics , Arabidopsis Proteins/metabolism , MADS Domain Proteins/metabolism , Repressor Proteins/metabolism , Seedlings/genetics , Seeds/genetics
12.
Nucleic Acids Res ; 49(1): 98-113, 2021 01 11.
Article in English | MEDLINE | ID: mdl-33270882

ABSTRACT

The Polycomb repressive complex 2 (PRC2) catalyzes histone H3 Lys27 trimethylation (H3K27me3) to repress gene transcription in multicellular eukaryotes. Despite its importance in gene silencing and cellular differentiation, how PRC2 is recruited to target loci is still not fully understood. Here, we report genome-wide evidence for the recruitment of PRC2 by the transcriptional repressors VIVIPAROUS1/ABI3-LIKE1 (VAL1) and VAL2 in Arabidopsis thaliana. We show that the val1 val2 double mutant possesses somatic embryonic phenotypes and a transcriptome strikingly similar to those of the swn clf double mutant, which lacks the PRC2 catalytic subunits SWINGER (SWN) and CURLY LEAF (CLF). We further show that VAL1 and VAL2 physically interact with SWN and CLF in vivo. Genome-wide binding profiling demonstrated that they colocalize with SWN and CLF at PRC2 target loci. Loss of VAL1/2 significantly reduces SWN and CLF enrichment at PRC2 target loci and leads to a genome-wide redistribution of H3K27me3 that strongly affects transcription. Finally, we provide evidence that the VAL1/VAL2-RY regulatory system is largely independent of previously identified modules for Polycomb silencing in plants. Together, our work demonstrates an extensive genome-wide interaction between VAL1/2 and PRC2 and provides mechanistic insights into the establishment of Polycomb silencing in plants.


Subject(s)
Arabidopsis Proteins/metabolism , Arabidopsis/genetics , Gene Expression Regulation, Plant , Gene Silencing , Polycomb Repressive Complex 2/metabolism , Repressor Proteins/metabolism , Arabidopsis/metabolism , Arabidopsis Proteins/genetics , Epigenetic Repression , Gene Ontology , Histones/metabolism , Homeodomain Proteins/genetics , Homeodomain Proteins/metabolism , Polycomb Repressive Complex 2/genetics , Protein Binding , Protein Interaction Mapping , Repressor Proteins/deficiency , Repressor Proteins/genetics , Response Elements/genetics , Transcription Factors/genetics , Transcription Factors/metabolism , Transcription, Genetic
13.
Plant Physiol ; 184(4): 1969-1978, 2020 12.
Article in English | MEDLINE | ID: mdl-33037128

ABSTRACT

Seed dormancy is an adaptive trait that is crucial to plant survival. Abscisic acid (ABA) is the primary phytohormone that induces seed dormancy. However, little is known about how the level of ABA in seeds is determined. Here we show that the Arabidopsis (Arabidopsis thaliana) H3K27me3 demethylase RELATIVE OF EARLY FLOWERING6 (REF6) suppresses seed dormancy by inducing ABA catabolism in seeds. Seeds of the ref6 loss-of-function mutants displayed enhanced dormancy that was associated with increased endogenous ABA content. We further show that the transcripts of two genes key to ABA catabolism, CYP707A1 and CYP707A3, but not genes involved in ABA biosynthesis, were significantly reduced in ref6 mutants during seed development and germination. In developing siliques, REF6 bound directly to CYP707A1 and CYP707A3, and was responsible for reducing their H3K27me3 levels. Genetic analysis demonstrated that the enhanced seed dormancy and ABA concentration in ref6 depended mainly on the reduced expression of CYP707A1 and CYP707A3 Conversely, overexpression of CYP707A1 could offset the enhanced seed dormancy of ref6 Taken together, our results revealed an epigenetic regulation mechanism that is involved in the regulation of ABA content in seeds.


Subject(s)
Abscisic Acid/metabolism , Arabidopsis/genetics , Arabidopsis/physiology , Epigenesis, Genetic , Germination/genetics , Plant Dormancy/genetics , Plant Dormancy/physiology , Gene Expression Regulation, Plant , Genes, Plant
14.
Nat Plants ; 6(8): 996-1007, 2020 08.
Article in English | MEDLINE | ID: mdl-32747760

ABSTRACT

Switch defective/sucrose non-fermentable (SWI/SNF) chromatin remodelling complexes are multi-protein machineries that control gene expression by regulating chromatin structure in eukaryotes. However, the full subunit composition of SWI/SNF complexes in plants remains unclear. Here we report that in Arabidopsis thaliana, two homologous glioma tumour suppressor candidate region domain-containing proteins, named BRAHMA-interacting proteins 1 (BRIP1) and BRIP2, are core subunits of plant SWI/SNF complexes. brip1 brip2 double mutants exhibit developmental phenotypes and a transcriptome remarkably similar to those of BRAHMA (BRM) mutants. Genetic interaction tests indicated that BRIP1 and BRIP2 act together with BRM to regulate gene expression. Furthermore, BRIP1 and BRIP2 physically interact with BRM-containing SWI/SNF complexes and extensively co-localize with BRM on chromatin. Simultaneous mutation of BRIP1 and BRIP2 results in decreased BRM occupancy at almost all BRM target loci and substantially reduced abundance of the SWI/SNF assemblies. Together, our work identifies new core subunits of BRM-containing SWI/SNF complexes in plants and uncovers the essential role of these subunits in maintaining the abundance of SWI/SNF complexes in plants.


Subject(s)
Arabidopsis Proteins/metabolism , Chromatin Assembly and Disassembly , Chromatin/metabolism , Nuclear Proteins/metabolism , Pyruvate Kinase/metabolism , Adenosine Triphosphatases/metabolism , Arabidopsis/metabolism , Chromosomal Proteins, Non-Histone , Transcription Factors, General
15.
J Am Chem Soc ; 141(21): 8407-8411, 2019 May 29.
Article in English | MEDLINE | ID: mdl-31083914

ABSTRACT

Hydrogenated black TiO2 is receiving ever-increasing attention, primarily due to its ability to capture low-energy photons in the solar spectrum and its highly efficient redox reactivity for solar-driven water splitting. However, in-depth physical insight into the redox reactivity is still missing. In this work, we conducted a density functional theory study with Hubbard U correction (DFT+U) based on the model obtained from spectroscopic and aberration-corrected scanning transmission electron microscopy (AC-STEM) characterizations to reveal the synergy among H heteroatoms located at different surface sites where the six-coordinated Ti (Ti6C) atom is converted from an inert trapping site to a site for the interchange of photoexcited electrons. This in-depth understanding may be applicable to the rational design of highly efficient solar-light-harvesting catalysts.

16.
Angew Chem Int Ed Engl ; 57(28): 8550-8554, 2018 07 09.
Article in English | MEDLINE | ID: mdl-29676041

ABSTRACT

Introducing band gap states to TiO2 photocatalysts is an efficient strategy for expanding the range of accessible energy available in the solar spectrum. However, few approaches are able to introduce band gap states and improve photocatalytic performance simultaneously. Introducing band gap states by creating surface disorder can incapacitate reactivity where unambiguous adsorption sites are a prerequisite. An alternative method for introduction of band gap states is demonstrated in which selected heteroatoms are implanted at preferred surface sites. Theoretical prediction and experimental verification reveal that the implanted heteroatoms not only introduce band gap states without creating surface disorder, but also function as active sites for the CrVI reduction reaction. This promising approach may be applicable to the surfaces of other solar harvesting materials where engineered band gap states could be used to tune photophysical and -catalytic properties.

17.
Front Plant Sci ; 8: 28, 2017.
Article in English | MEDLINE | ID: mdl-28167952

ABSTRACT

Nitrogen (N) and silicon (Si) are two important nutritional elements required for plant growth, and both impact host plant resistance toward insect herbivores. The interaction between the two elements may therefore play a significant role in determining host plant resistance. We investigated this interaction in rice (Oryza sativa L.) and its effect on resistance to the herbivore brown planthopper Nilaparvata lugens (BPH). Our results indicate that high-level (5.76 mM) N fertilization reduced Si accumulation in rice leaves, and furthermore, this decrease was likely due to decreased expression of Si transporters OsLsi1 and OsLsi2. Conversely, reduced N accumulation was observed at high N fertilization levels when Si was exogenously provided, and this was associated with down-regulation of OsAMT1;1 and OsGS1;1, which are involved in ammonium uptake and assimilation, respectively. Under lower N fertilization levels (0.72 and/or 1.44 mM), Si amendment resulted in increased OsNRT1:1, OsGS2, OsFd-GOGAT, OsNADH-GOGAT2, and OsGDH2 expression. Additionally, bioassays revealed that high N fertilization level significantly decreased rice resistance to BPH, and the opposite effect was observed when Si was provided. These results provide additional insight into the antagonistic interaction between Si and N accumulation in rice, and the effects on plant growth and susceptibility to herbivores.

18.
Chem Commun (Camb) ; 51(90): 16244-6, 2015 Nov 21.
Article in English | MEDLINE | ID: mdl-26399299

ABSTRACT

Mesoporous g-C3N4 has been obtained by a facile sucrose-mediated approach via thermal condensation of sucrose and melamine for the first time. The mesoporous g-C3N4 presents a much higher BET surface area and displays highly enhanced photocatalytic H2 evolution performance.

19.
Chem Commun (Camb) ; 51(31): 6824-7, 2015 Apr 21.
Article in English | MEDLINE | ID: mdl-25786546

ABSTRACT

Carbonized polydopamine-graphitic carbon nitride (C-PDA-g-C3N4) composites have been synthesised via in situ polymerization of dopamine (DA) on the surface of melamine followed by carbonization and condensation for the first time. The obtained C-PDA-g-C3N4 composites display enhanced crystallinity and superior photocatalytic performance.

20.
Chem Commun (Camb) ; 51(2): 425-7, 2015.
Article in English | MEDLINE | ID: mdl-25408286

ABSTRACT

A facile sulfur-bubble template-mediated synthesis of uniform porous g-C3N4 has been developed for the first time. The obtained sulfur-mediated g-C3N4 presents a uniform porous structure with higher BET surface area and displays superior photocatalytic performance compared with pure g-C3N4.

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