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Advances of graphdiyne-supported metal catalysts in thermocatalytic reactions

Nano Research 2024年第4期17卷 2223-2233页

作者： Jia Yu Yida Yang Yuliang Li Changyan Cao Weiguo Song Beijing National Laboratory for molecular sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of Molecular Nanostructures and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical sciences University of Chinese Academy of SciencesBeijing 100049China Beijing National Laboratory for molecular sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of organic solidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Supported metal catalysts are widely used in the modern chemical industry.The electronic interaction between supports and active components is of great significance for heterogeneous catalysis.Graphdiyne(GDY),a new type of carbon allotrope with sp-hybridized carbon atoms,πconjugate structure,and electron transmission capability,is a promising candidate as catalyst support.Recent years have witnessed the rapid progress of GDY-supported metal catalysts for different catalysis reactions.Considering that most processes in the current chemical industry are thermocatalytic reactions,we herein give an overview about the advances and particular characteristics of GDY-supported catalysts in these reactions.The geometric structure and electronic properties of GDY are first introduced.Then,the synthesis methods for GDY-supported metal catalysts and their applications in thermocatalytic reactions are discussed,in which the effect of electronic interaction on catalytic performance is highlighted.Finally,the current challenges and future directions of GDY-supported metal catalysts for thermocatalysis are proposed.It is expected that this review will enrich our understanding of the advances of GDY as a superior support for metal catalysts in thermocatalytic reactions.

关键词： graphdiyne metal catalysts thermocatalytic reactions heterogeneous catalysis

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C_(Ar)-Br bond cleavage via cooperative EnT/NHC catalysis: mild access to indolines

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Science China Chemistry 2024年第3期67卷 922-927页

作者： Yi-Xiong Dong Cao-Bo Li Ming-Lei Jin Zhong-Hua Gao Song Ye Beijing National Laboratory for molecular sciences CAS Key Laboratory of Molecular Recognition and FunctionCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of sciences Beijing 100049China

The cooperative visible-light mediated and NHC-catalyzed dearomative arylation-acylation of N-(2-bromobenzoyl)indoles with aldehydes was developed, affording the corresponding highly functionalized polycyclic indolines in moderate to good yields with exclusive diastereoselectivities. Mechanism investigations support the activation of CAr-Br bond via visible-light mediated energy transfer(EnT) and the following single-electron-transfer(SET) with Breslow intermediate under NHC catalysis to give key aryl radical and ketyl radical. This protocol demonstrates the cleavage of CAr-Br bond under mild cooperative EnT/NHC catalysis.

关键词： energy transfer N-heterocyclic carbenes photocatalysis aryl radicals indolines

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Multifunction-oriented high-mobility polymer semiconductors

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National Science Review 2024年第3期11卷 16-19页

作者： Mingliang Zhu Yunlong Guo Yunqi Liu Beijing National Laboratory for molecular sciences Organic Solids Laboratory Institute of Chemistry Chinese Academy of Sciences School of Chemical sciences University of Chinese Academy of Sciences

The discovery of conductive polyacetylene has initiated interdisciplinary research into condensed matter physics and synthetic chemistry in organic electronics. Unlike their inorganic and small-molecule counterparts, polymer semiconductors possess the inherent advantages of facile solution processing,large-area manufacturing, excellent mechanical strength and intrinsic flexibility.

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Bias distribution and regulation in photoelectrochemical overall water-splitting cells

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National Science Review 2024年第4期11卷 141-150页

作者： Kun Dang Siqin Liu Lei Wu Daojian Tang Jing Xue Jiaming Wang Hongwei Ji Chuncheng Chen Yuchao Zhang Jincai Zhao Key Laboratory of Photochemistry CAS ResearchEducation Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of sciences

The water oxidation half-reaction at anodes is always considered the rate-limiting step of overall water splitting（OWS）,but the actual bias distribution between photoanodes and cathodes of photoelectro chemical（PEC） OWS cells has not been investigated systematically.In this work,we find that,for PEC cells consisting of photoanodes（nickel-modified n-Si [Ni/n-Si] and α-Fe2O3） with low photovoltage(Vph 1V,the bias required for cathode activation can be significantly reduced,exhibiting a kinetics-controlled characteristic.Further investigations show that the bias distribution can be regulated by tuning the electrolyte pH and using alternative half-reaction couplings.Accordingly,a volcano plot is presented for the rational design of the overall reactions and unbiased PEC cells.Motivated by this,an unbiased PEC cell consisting of a simple Ni/n-Si photoanode and Pt cathode is assembled,delivering a photo current density of 5.3±0.2 mA cm-2.

关键词： photoelectrochemistry overall reaction cell bias distribution photoanode water splitting

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Solid-state lithium-ion batteries for grid energy storage:opportunities and challenges

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Science China Chemistry 2024年第1期67卷 43-66页

作者： Xin Chang Yu-Ming Zhao Boheng Yuan Min Fan Qinghai Meng Yu-Guo Guo Li-Jun Wan CAS Key Laboratory of molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of sciences Beijing 100049China

The energy crisis and environmental pollution drive more attention to the development and utilization of renewable energy.Considering the capricious nature of renewable energy resource,it has difficulty supplying electricity directly to consumers stably and efficiently,which calls for energy storage systems to collect energy and release electricity at peak periods.Due to their flexible power and energy,quick response,and high energy conversion efficiency,lithium-ion batteries stand out among multiple energy storage technologies and are rapidly deployed in the grid.Pursuing superior performance and ensuring the safety of energy storage systems,intrinsically safe solid-state electrolytes are expected as an ideal alternative to liquid electrolytes.In this review,we systematically evaluate the priorities and issues of traditional lithium-ion batteries in grid energy storage.Beyond lithium-ion batteries containing liquid electrolytes,solid-state lithium-ion batteries have the potential to play a more significant role in grid energy storage.The challenges of developing solid-state lithium-ion batteries,such as low ionic conductivity of the electrolyte,unstable electrode/electrolyte interface,and complicated fabrication process,are discussed in detail.Additionally,the safety of solid-state lithium-ion batteries is re-examined.Following the obtained insights,inspiring prospects for solid-state lithium-ion batteries in grid energy storage are depicted.

关键词： lithium-ion batteries grid energy storage solid-state electrolytes interface stability

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Asymmetric Hydrogenation of Phenanthridines with Chiral Boranes

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Chinese Journal of Chemistry 2024年第6期42卷 631-635页

作者： Guangyu Cui Xiangqing Feng Haifeng Du Beijing National Laboratory for molecular sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190 China University of Chinese Academy of sciences Beijing100049 China

The asymmetric hydrogenation of N-heteroarenes provides an efficient method for the synthesis of optically active cyclic secondary amines.In this paper,we described an asymmetric hydrogenation of phenanthridines using a chiral mono-alkene-derived borane.A variety of dihydrophenanthridines were furnished in high yields with up to 93%ee.The current catalytic system was very sensitive for the steric hindrance of phenanthridines.Bulky substituents at one phenyl group of phenanthridines were required to obtain the high enantioselectivity.But large substituents on the carbon of the C=N bonds would diminish the reactivity sharply.

关键词： Asymmetric catalysis Hydrogenation Nitrogen heterocycles Phenanthridines Frustrated Lewis pairs Chiral boranes

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FKF1b controls reproductive transition associated with adaptation to geographical distribution in maize

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Journal of integrative Plant Biology 2024年第5期66卷 943-955页

作者： Suhui Chen Shan Gao Dongyang Wang Jie Liu Yingying Ren Zhihan Wang Xin Wei Qin Wang Xuehui Huang Shanghai Key Laboratory of Plant molecular sciences College of Life SciencesShanghai Normal UniversityShanghai 200234China

Maize(Zea mays subspecies mays)is an important commercial crop across the world,and its flowering time is closely related to grain yield,plant cycle and latitude adaptation.FKF1 is an essential clock-regulated blue-light receptor with distinct functions on flowering time in plants,and its function in maize remains unclear.In this study,we identified two FKF1 homologs in the maize genome,named ZmFKF1a and ZmFKF1b,and indicated that ZmFKF1a and ZmFKF1b independently regulate reproductive transition through interacting with ZmCONZ1 and ZmGI1 to increase the transcription levels of ZmCONZ1 and ZCN8.We demonstrated that ZmFKF1b underwent artificial selection during modern breeding in China probably due to its role in geographical adaptation.Furthermore,our data suggested that ZmFKF1bHap_C7 may be an elite allele,which increases the abundance of ZmCONZ1 mRNA more efficiently and adapt to a wider range of temperature zone than that of ZmFKF1bHap_Z58 to promote maize floral transition.It extends our understanding of the genetic diversity of maize flowering.This allele is expected to be introduced into tropical maize germplasm to enrich breeding resources and may improve the adaptability of maize at different climate zones,especially at temperate region.

关键词： flowering geographical distribution maize ZmFKF1

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How plants sense and respond to osmotic stress

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Journal of integrative Plant Biology 2024年第3期66卷 394-423页

作者： Bo Yu Dai-Yin Chao Yang Zhao Shanghai Center for Plant Stress Biology CAS Center for Excellence in Molecular Plant SciencesThe Chinese Academy of SciencesShanghai 200032China Key Laboratory of Plant Carbon Capture The Chinese Academy of SciencesShanghai 200032China National Key Laboratory of Plant molecular Genetics CAS Center for Excellence in Molecular Plant SciencesInstitute of Plant Physiology and EcologyThe Chinese Academy of SciencesShanghai 200032China University of Chinese Academy of sciences Beijing 100049China

Drought is one of the most serious abiotic stresses to land plants.Plants sense and respond to drought stress to survive under water deficiency.Scientists have studied how plants sense drought stress,or osmotic stress caused by drought,ever since Charles Darwin,and gradually obtained clues about osmotic stress sensing and signaling in plants.Osmotic stress is a physical stimulus that triggers many physiological changes at the cellular level,including changes in turgor,cell wall stiffness and integrity,membrane tension,and cell fluid volume,and plants may sense some of these stimuli and trigger downstream responses.In this review,we emphasized water potential and movements in organisms,compared putative signal inputs in cell wall-containing and cell wall-free organisms,prospected how plants sense changes in turgor,membrane tension,and cell fluid volume under osmotic stress according to advances in plants,animals,yeasts,and bacteria,summarized multilevel biochemical and physiological signal outputs,such as plasma membrane nanodomain formation,membrane water permeability,root hydrotropism,root halotropism,Casparian strip and suberin lamellae,and finally proposed a hypothesis that osmotic stress responses are likely to be a cocktail of signaling mediated by multiple osmosensors.We also discussed the core scientific questions,provided perspective about the future directions in this field,and highlighted the importance of robust and smart root systems and efficient source-sink allocations for generating future high-yield stress-resistant crops and plants.

关键词： cell volume drought membrane tension osmotic stress turgor

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Chemoproteomics reveals the epoxidase enzyme for the biosynthesis of camptothecin in Ophiorrhiza pumila

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Journal of integrative Plant Biology 2024年第6期66卷 1044-1047页

作者： Tong Zhang Yan Wang Shiwen Wu Ernuo Tian Chengshuai Yang Zhihua Zhou Xing Yan Pingping Wang CAS-Key Laboratory of Synthetic Biology CAS Center for Excellence in Molecular Plant Sciences Chinese Academy of Sciences University of Chinese Academy of sciences

Camptothecin is one of the most commonly used anticancer drugs worldwide, yet the downstream biosynthetic route from strictosidine to camptothecin has remained unclear for more than half a century. Here,we searched for proteins involved in camptothecin biosynthesis from the camptothecin-producing plant Ophiorrhiza pumila by chemoproteomics and identified Op CYP716E111.

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OsPDR20 is an ABCG metal transporter regulating cadmium accumulation in rice

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Journal of Environmental sciences 2024年第2期136卷 21-34页

作者： He Li Chao Li Di Sun Zhi Min Yang Department of Biochemistry and molecular Biology College of Life SciencesNanjing Agricultural UniversityNanjing 210095China

Cadmium(Cd)is a non-essential toxic heavy metal,seriously posing high environmental risks to human health.Digging genetic resources relevant to functional genes is important for understanding the metal absorption and accumulation in crops and bioremediation of Cd-polluted environments.This study investigated a functionally uncharacterized ATP binding cassette transporter G family(ABCG)gene encoding a Pleiotropic Drug Resistance 20(PDR20)type metal transporter which is localized to the plasma membrane of rice.OsPDR20 was transcriptionally expressed in almost all tissues and organs in lifespan and was strongly induced in roots and shoots of young rice under Cd stress.Ectopic expression of OsPDR20 in a yeast mutant ycf1 sensitive to Cd conferred cellular tolerance with less Cd accumulation.Knockdown of OsPDR20 by RNA interference(RNAi)moderately attenuated root/shoot elongation and biomass,with reduced chlorophylls in rice grown under hydroponic medium with 2 and 10μmol/L Cd,but led to more Cd accumulation.A field trial of rice grown in a realistic Cd-contaminated soil(0.40 mg/kg)showed that RNAi plants growth and development were also compromised compared to wild-type(WT),with smaller panicles and lower spikelet fertility but little effect on yield of grains.However,OsPDR20 suppression resulted in unexpectedly higher levels of Cd accumulation in rice straw including lower leaves and culm and grain.These results suggest that OsPDR20 is actively involved in Cd accumulation and homeostasis in rice crops.The increased Cd accumulation in the RNAi plants has the potential application in phytoremediation of Cd-polluted wetland soils.

关键词： Rice ABCG transporter Cadmium accumulation Phytoremediation

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