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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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Discontinuous phase diagram of amorphous carbons

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National Science Review 2024年第4期11卷 164-171页

作者： YinBo Zhu ZhouYu Fang ZhongTing Zhang HengAn wu cas key laboratory of Mechanical Behavior and Design of Materials Department of Modern MechanicsUniversity of Science and Technology of China State key laboratory of Nonlinear Mechanics Institute of Mechanics Chinese Academy of Sciences

The short-range order and medium-range order of amorphous carbons demonstrated in experiments allow us to rethink whether there exist intrinsic properties hidden by atomic disordering. Here we presented six representative phases of amorphous carbons（0.1–3.4 g/cm3）, namely, disordered graphene network（DGN）, high-density amorphous carbon（HDAC）, amorphous diaphite（a-DG）, amorphous diamond（a-D）, paracrystalline diamond（p-D）, and nano-polycrystalline diamond（NPD）, respectively, classified by their topological features and microstructural characterizations that are comparable with experiments. To achieve a comprehensive physical landscape for amorphous carbons, a phase diagram was plotted in the sp3/sp2versus density plane, in which the counterintuitive discontinuity originates from the inherent difference in topological microstructures, further guiding us to discover a variety of phase transitions among different amorphous carbons. Intriguingly, the power law, log（sp3/sp2） ∝ ρn, hints at intrinsic topology and hidden order in amorphous carbons, providing an insightful perspective to reacquaint atomic disorder in non-crystalline carbons.

关键词： amorphous carbons disordered carbons phase diagram microstructural topology phase transition

Inducing mitochondriopathy-like damages by transformable nucleopeptide nanoparticles for targeted therapy of bladder cancer

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National Science Review 2024年第4期11卷 216-227页

作者： Da-Yong Hou Ni-Yuan Zhang Lu Wang Mei-Yu Lv Xiang-Peng Li Peng Zhang Yue-Ze Wang Lei Shen Xiu-Hai wu Bo Fu Peng-Yu Guo Zi-Qi Wang Dong-Bing Cheng Hao Wang Wanhai Xu NHC and CAMS key laboratory of Molecular Probe and Targeted Theranostics Heilongjiang Key Laboratory of Scientific Research in Urology Harbin Medical University Department of Urology Harbin Medical University Cancer Hospital cas key laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST) School of Chemistry Chemical Engineering & Life Science Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases Wuhan University of Technology

Mitochondriopathy inspired adenosine triphosphate(ATP) depletions have been recognized as a powerful way for controlling tumor growth. Nevertheless, selective sequestration or exhaustion of ATP under complex biological environments remains a prodigious challenge. Harnessing the advantages of in vivo self-assembled nanomaterials, we designed an Intracellular ATP Sequestration(IAS) system to specifically construct nanofibrous nanostructures on the surface of tumor nuclei with exposed ATP binding sites,leading to highly efficient suppression of bladder cancer by induction of mitochondriopathy-like damages.Briefly, the reported transformable nucleopeptide(NLS-FF-T) self-assembled into nuclear-targeted nanoparticles with ATP binding sites encapsulated inside under aqueous conditions. By interaction with KPNA2, the NLS-FF-T transformed into a nanofibrous-based ATP trapper on the surface of tumor nuclei,which prevented the production of intracellular energy. As a result, multiple bladder tumor cell lines(T24,EJ and RT-112) revealed that the half-maximal inhibitory concentration(IC50) of NLS-FF-T was reduced by approximately 4-fold when compared to NLS-T. Following intravenous administration, NLS-FF-T was found to be dose-dependently accumulated at the tumor site of T24 xenograft mice. More significantly, this IAS system exhibited an extremely antitumor efficacy according to the deterioration of T24 tumors and simultaneously prolonged the overall survival of T24 orthotopic xenograft mice. Together, our findings clearly demonstrated the therapeutic advantages of intracellular ATP sequestration-induced mitochondriopathy-like damages, which provides a potential treatment strategy for malignancies.

关键词： self-assembly nucleopeptide nanomaterial bladder cancer mitochondriopathy

Sustainable, thermoplastic and hydrophobic coating from natural cellulose and cinnamon to fabricate eco-friendly catering packaging

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Green Energy & Environment 2024年第5期9卷 927-936页

作者： Rumeng Xu Chunchun Yin Jingxuan You Jinming Zhang Qinyong Mi Jin wu Jun Zhang cas key laboratory of Engineering Plastics Institute of ChemistryChinese Academy of Sciences(CAS)Beijing100190China University of Chinese Academy of Sciences Beijing100049China

Non-degradable polymers cause serious environmental pollution problem,such as the widely-used while unrecyclable coatings which signiﬁcantly affect the overall degradation performance of products.It is imperative and attractive to develop biodegradable functional coatings.Herein,we proposed a novel strategy to successfully prepare biodegradable,thermoplastic and hydrophobic coatings with high transparence and biosafety by weakening the interchain interactions between cellulose chain.The natural cellulose and cinnamic acid were as raw materials.Via reducing the degree of polymerization(DP)of cellulose and regulating the degree of substitution(DS)of cinnamate moiety,the obtained cellulose cinnamate(CC)exhibited not only the thermalﬂow behavior but also good biodegradability,which solves the conﬂict between the thermoplasticity and biodegradability in cellulose-based materials.The glass transition temperature(T_(g))and thermalﬂow temperature(T_(f))of the CC could be adjusted in a range of 150–200℃ and 180–210℃,respectively.The CC with DS<1.2 and DP≤100 degraded more than 60%after an enzyme treatment for 7 days,and degraded more than 80%after a composting treatment for 42 days.Furthermore,CC had no toxicity to human epidermal cells even at a high concentration(0.5 mg mL^(-1)).In addition,CC could be easily fabricated into multifunctional coating with high hydrophobicity,thermal adhesion and high transparence.Therefore,after combining with cellophane and paperboard,CC coating with low DP and DS could be used to prepare fully-biodegradable heat-sealing packaging,art paper,paper cups,paper straws and food packaging boxes.

关键词： Thermoplastic coating Bio-degradable adhesive Natural products Cellulose Eco-friendly packaging

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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

A STABILITY RESULT FOR TRANSLATINGSPACELIKE GRAPHS IN LORENTZ MANIFOLDS

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Acta Mathematica Scientia 2024年第2期44卷 474-483页

作者：高雅毛井吴传喜 Faculty of mathematics and Statistics Key Laboratory of Applied Mathematics of Hubei ProvinceHubei UniversityWuhan430062China

In this paper,we investigate spacelike graphs defined over a domain Ω⊂M^(n) in the Lorentz manifold M^(n)×ℝ with the metric−ds^(2)+σ,where M^(n) is a complete Riemannian n-manifold with the metricσ,Ωhas piecewise smooth boundary,and ℝ denotes the Euclidean 1-space.We prove an interesting stability result for translating spacelike graphs in M^(n)×ℝ under a conformal transformation.

关键词： mean curvature flow spacelike graphs translating spacelike graphs maximal spacelike graphs constant mean curvature Lorentz manifolds

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Chain Dynamics Heterogeneity in Plasticized Poly(vinyl butyral)(PVB) as Elucidated by Solid-State NMR

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Chinese Journal of Polymer Science 2024年第1期42卷 113-124,I0010页

作者： Jing Lv Xu Chen Zi-Shuo wu Ya-Hui Li Wei Chen National Synchrotron Radiation laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer FilmCAS Key Laboratory of Soft Matter ChemistryUniversity of Scienceand Technology of ChinaHefei 230026China

The chain dynamics heterogeneity of the poly(vinyl butyral)(PVB) plasticized by triethylene glycol bis(2-ethylhexa noate)(TEG-EH) was investigated by various solid-state NMR techniques.The plasticized PVB shows two domains in distinct molecular dynamics differences,namely,rigid and soft domains,where the latter is the plasticizer-rich domain.The time domain low field NMR was first used to investigate the dynamics heterogeneity of the plasticized PVB,and the results show the decreasing activated energy of components in the soft domain of plasticized PVB(E_a=20.2 kJ/mol) as compared with that of the pristine one(E_a=24.3 kJ/mol).Detailed dynamics heterogeneity was obtained by high-field NMR with site-specific features.The quadrupole-echo ~2H-NMR was adopted to elucidate the dynamics heterogeneity of the vinyl alcohol(VA) units,where only the hydroxyl group of VA is deuterated.The ~1H-^(13)C WISE NMR spectra show that there is not much difference in the mobility of the VB unit in PVB with and without plasticizer,whereas the glass transition temperature differed by approximately 53℃.This is further supported by Torchia's T_1 relaxation measurements.The origin of such an unusual phenomenon is attributed to the critical role of the remaining VA(~22%) in the soft domain,where the VA units locally aggregate through hydrogen bonding.Also,the existence of a mobility gradient in the VB unit has been demonstrated.Moreover,the mobility difference for VB with different stereo-geometry(meso or racemic conformation) is observed for the first time.This indicates the importance of modulating the ratio of meso over racemic VB for controlling the macroscopic perfo rmance of PVB.

关键词： Poly(vinyl butyral) Dynamics heterogeneity Plasticizer Solid state NMR

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Regulation of the quantum barrier and carrier transport toward high-efficiency quasi-2D Dion-Jacobson tin perovskite solar cells

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Journal of Energy Chemistry 2024年第8期95卷 200-207页

作者： Huanhuan Yao Chang Shi Tai wu Shurong Wang Mingyu Yin Liming Ding Yong Hua Feng Hao School of Materials and Energy University of Electronic Science and Technology of China College of Chemistry and Molecular Engineering Peking University Yunnan key laboratory for Micro/Nano Materials & Technology School of Materials and Energy Yunnan University Center for Excellence in Nanoscience (cas) Key Laboratory of Nanosystem and Hierarchical Fabrication (CAS) National Center for Nanoscience and Technology

Quasi-2D Dion-Jacobson（DJ） tin halide perovskite has attracted much attention due to its elimination of Van der Waals gap and enhanced environmental stability.However,the bulky organic spacers usually form a natural quantum well structure,which brings a large quantum barrier and poor film quality,further limiting the carrier transport and device performance.Here,we designed three organic spacers with different chain lengths(ethylenediamine（EDA）,1,3-propanediamine（PDA）,and 1,4-butanediamine（BDA）) to investigate the quantum barrier dependence.Theoretical and experimental characterizations indicate that EDA with short chain can reduce the lattice distortion and dielectric confinement effect,which is beneficial to the effective dissociation of excitons and the inhibition of trap-free non-radiative relaxation.In addition,EDA cation shows strong interaction with the inorganic octahedron,realizing large aggregates in precursor solution and high-quality films with improved structural stability.Furthermore,femtosecond transient absorption proves that EDA cations can also weaken the formation of small n-phases with large quantum barrier to achieve effective carrier transport between different nphases.Finally,the quasi-2D DJ（EDA）FA9Sn10I31solar cells achieves a 7.07% power conversion efficiency with good environment stability.Therefore,this work sheds light on the regulation of the quantum barrier and carrier transport through the chain length of organic spacer for qua si-2D DJ lead-free perovskites.

关键词： Carrier transport Chain lengths Lattice distortion Organic spacers Quantum well

Persistence of charge density wave against variation of band structures in V_(x)Ti_(1−x)Se_(2)(x=0–0.1)

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Nano Research 2024年第3期17卷 2129-2135页

作者： Zhanfeng Liu Tongrui Li wen Zhu Hongwei Shou Mukhtar Lawan Adam Qilong Cui Yuliang Li Sheng Wang Yunbo wu Hongen Zhu Yi Liu Shuangming Chen Xiaojun wu Shengtao Cui Li Song Zhe Sun National Synchrotron Radiation laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230029China cas key laboratory of Strongly-coupled Quantum Matter Physics University of Science and Technology of ChinaHefei 230026China Collaborative Innovation Center of Advanced Microstructures Nanjing 210093China State key laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China School of Chemistry and Materials Sciences CAS Key Laboratory of Materials for Energy Conversionand CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230026China School Zhejiang Institute of Photonelectronics Jinhua 321004China

Charge density wave(CDW)is a phenomenon that occurs in materials,accompanied by changes in their intrinsic electronic properties.The study of CDW and its modulation in materials holds tremendous significance in materials research,as it provides a unique approach to controlling the electronic properties of materials.TiSe_(2) is a typical layered material with a CDW phase at low temperatures.Through V substitution for Ti in TiSe_(2),we tuned the carrier concentration in V_(x)Ti_(1-x)Se_(2) to study how its electronic structures evolve.Angle-resolved photoemission spectroscopy(ARPES)shows that the band-folding effect is sustained with the doping level up to 10%,indicating the persistence of the CDW phase,even though the band structure is strikingly different from that of the parent compound TiSe_(2).Though CDW can induce the band fold effect with a driving force from the perspective of electronic systems,our studies suggest that this behavior could be maintained by lattice distortion of the CDW phase,even if band structures deviate from the electron-driven CDW scenario.Our work provides a constraint for understanding the CDW mechanism in TiSe_(2),and highlights the role of lattice distortion in the band-folding effect.

关键词： charge density wave band structure lattice distortion