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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 *** 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 *** investigations show that the bias distribution can be regulated by tuning the electrolyte pH and using alternative half-reaction ***,a volcano plot is presented for the rational design of the overall reactions and unbiased PEC *** 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

Visible-light-induced organocatalyzed C（sp2）–H bond functionalization of 1,3-azoles with trifluoroacetylsilanes

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Science China Chemistry 2024年第11期67卷 3662-3668页

作者： Zhengyu Li Zeguo Zhang Zhihan Zhang Gang Zhou Yizhi Zhang Shanshan Liu Xiao Shen The Institute for Advanced Studies Engineering Research Center of Organosilicon Compounds & Materials Ministry of EducationWuhan University College of Chemistry Central China Normal University

Previous carbene insertion to C–H bonds of 1,3-azoles relied on metal carbene species. Herein, we report a metal-free C（sp2）–H bond functionalization of 1,3-azoles with trifluoroacetylsilanes. The reaction features mild conditions, broad substrate scope and wide functional group tolerance. The mechanistic study supports that the success of the reaction is probably attributed to the dual roles of trifluoroacetylsilanes under the photocatalyzed conditions: generating carbenes which undergo cyclopropanation and generating biradicals which promote ring-opening aromatization of the in situ generated fused cyclopropanes.

关键词： C(sp2)–H bond functionalization carbenes biradicals cyclopropanation brook rearrangement

Targeting lncRNA16 by GalNAc-siRNA conjugates facilitates chemotherapeutic sensibilization via the HBB/NDUFAF5/ROS pathway

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Science China(Life Sciences) 2024年第4期67卷 663-679页

作者： Yanfang Liu Yan Wang Bing Liu Wenzhong Liu Yuanyuan Ma Yiren Cao Shi Yan Panpan Zhang Lixin Zhou Qimin Zhan Nan Wu Key Laboratory of Carcinogenesis and Translational research(Ministry of education/Beijing) Department of Thoracic Surgery IIPeking University Cancer Hospital and InstituteBeijing 100142China Key Laboratory of Carcinogenesis and Translational research(Ministry of education/Beijing) Laboratory of Molecular OncologyPeking University Cancer Hospital and InstituteBeijing 100142China Key Laboratory of Carcinogenesis and Translational research(Ministry of education/Beijing) Department of Thoracic Oncology IIPeking University Cancer Hospital and InstituteBeijing 100142China Key Laboratory of Carcinogenesis and Translational research(Ministry of education) Department of PathologyPeking University Cancer Hospital and InstituteBeijing 100142China Peking University International Cancer Institute Beijing 100191China Institute of Cancer research Shenzhen Bay LaboratoryShenzhen 518132China

Chemoresistance is a significant barrier to effective cancer *** mechanisms for chemoresistance include reactive oxygen species(ROS)accumulation and expression of chemoresistance-promoting ***,we report a novel function of lncRNA16 in the inhibition of ROS generation and the progression of *** analyzing the serum levels of lncRNA16 in a cohort of 35 patients with non-small cell lung cancer(NSCLC)and paired serum samples pre-and post-treatment from 10 NSCLC patients receiving neoadjuvant platinum-based chemotherapy,performing immunohistochemistry(IHC)assays on 188 NSCLC tumor samples,using comprehensive identification of RNA-binding proteins by mass spectrometry(ChIRP-MS)assays,as well as RNA immunoprecipitation(RIP)and RNA pull-down analyses,we discovered that patients with increased serum levels of lncRNA16 exhibited a poor response to platinum-based *** expression of hemoglobin subunit beta(HBB)and NDUFAF5 significantly increases with the development of ***16 binds to HBB and promotes HBB accumulation by inhibiting ***16 can also inhibit ROS generation via the HBB/NDUFAF5 axis and function as a scaffold to facilitate the colocalization of HBB and NDUFAF5 in the ***,preclinical studies in mouse models of chemo-resistant NSCLC have suggested that lncRNA16 targeting by trivalent N-acetylgalactosamine(GalNAc)-conjugated siRNA restores chemosensitivity and results in tumor growth inhibition with no detectable toxicity in ***,lncRNA16 is a promising therapeutic target for overcoming chemoresistance,and the combination of first-line platinum-based chemotherapy with lncRNA16 intervention can substantially enhance anti-tumor efficacy.

关键词： chemoresistance lncRNARNA interference ROs chemosensitizer

Enamel matrix proteins in promoting saliva lubrication

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Friction 2024年第10期12卷 2298-2312页

作者： Hujun WANG Yue TANG Haonan QIU Jingyang HU Yuan SU Jing ZHENG Zhongrong ZHOU Tribology research Institute School of Mechanical Engineering and Key Laboratory of Advanced Technologies of Materials(Ministry of Education)Southwest Jiaotong UniversityChengdu 610031China

Anti-wear performance of human enamel in the mouth is closely related to the lubrication of salivary *** is well known that the inorganic hydroxyapatite(HA)of the enamel plays an important role in the adsorption and pellicle-forming of salivary proteins on the enamel,but the role of enamel matrix proteins remains *** this study,the adsorption and lubrication behavior of salivary proteins on original,heated,and deproteinated enamel surfaces was comparatively investigated using an atomic force microscopy and nano-indentation/scratch *** with that on the original enamel surface,the adsorption and lubrication behavior of salivary proteins remains almost unchanged on the heated enamel surface(where the enamel matrix proteins are denatured but the size of HA crystalline nanoparticles keeps constant)but exhibits an obvious compromise on the deproteinated enamel surface(where the enamel matrix proteins are removed and agglomeration of HA crystallites occurs).The HA agglomeration weakens the electrostatic interaction of enamel surfaces with salivary proteins to cause a distinct negative influence on the adsorption and pellicle-forming of salivary ***,the negative effect is confirmed with a quartz crystal microbalance with *** summary,by regulating enamel nanostructure for appropriate electrostatic interactions between salivary proteins and enamel surfaces,the enamel matrix proteins play an essential role in the adsorption and pellicle-forming of salivary proteins on human enamel,and then contribute to saliva lubrication,which provides the enamel with an anti-wear *** findings will promote and assist the design of enamel-inspired anti-wear materials.

关键词： enamel matrix proteins hydroxyapatite(HA)crystalline nanoparticles salivary proteins adsorption lubrication

Data-driven Wasserstein distributionally robust chance-constrained optimization for crude oil scheduling under uncertainty

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Chinese Journal of Chemical Engineering 2024年第5期69卷 152-166页

作者： Xin Dai Liang Zhao Renchu He Wenli Du Weimin Zhong Zhi Li Feng Qian Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and TechnologyShanghai 200237China Engineering research Center of Process System Engineering Ministry of EducationEast China University of Science and TechnologyShanghai 200237China

Crude oil scheduling optimization is an effective method to enhance the economic benefits of oil *** uncertainties,including uncertain demands of crude distillation units(CDUs),might make the production plans made by the traditional deterministic optimization models infeasible.A data-driven Wasserstein distributionally robust chance-constrained(WDRCC)optimization approach is proposed in this paper to deal with demand uncertainty in crude oil ***,a new deterministic crude oil scheduling optimization model is developed as the basis of this *** Wasserstein distance is then used to build ambiguity sets from historical data to describe the possible realizations of probability distributions of uncertain demands.A cross-validation method is advanced to choose suitable radii for these ambiguity *** deterministic model is reformulated as a WDRCC optimization model for crude oil scheduling to guarantee the demand constraints hold with a desired high probability even in the worst situation in ambiguity *** proposed WDRCC model is transferred into an equivalent conditional value-at-risk representation and further derived as a mixed-integer nonlinear programming *** case studies from a real-world refinery are conducted to show the effectiveness of the proposed ***-of-sample tests demonstrate that the solution of the WDRCC model is more robust than those of the deterministic model and the chance-constrained model.

关键词： Distributions Model Optimization Crude oil scheduling Wasserstein distance Distributionally robust chance constraints

How the microenvironment dominated by the distance effect to regulate the FeN_(4)site ORR activity and selectivity?

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Nano research 2024年第6期17卷 5735-5741页

作者： Peng Li Qingfeng Guo Jianrui Zhang Ruilin Chen Shujiang Ding Yaqiong Su School of Chemistry Engineering Research Center of Energy Storage Materials and Devices of Ministry of EducationNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049China Huanghe Science and Technology College Zhengzhou 450063China General research Institute of Engineering of Gotion High-Tech Hefei 230041China

The distance effect of the doped heteroatoms away from the catalytic centers has rarely been *** this work,we conducted density functional theory calculations to thoroughly investigate the influence of heteroatom(N,P,B,and S atoms)doping distance on the oxygen reduction reaction(ORR)activity of graphene-based FeN_(4)*** uncovered a Sabatier-like relationship between heteroatom doping distance and ORR activity of FeN_(4)*** nearest doping does not significantly improve and even block the ORR activity of FeN_(4)*** ORR activity is achieved when the heteroatoms are 4-5Å(N,P,and S atoms)or 6-7Å(B atoms)away from the Fe *** of electronic structure indicates that distance effect can modulate the local chemical environment of Fe atoms,thereby account for the changes in ORR activity along with the doping distance and doping *** study provides insights into the influence of heteroatom doping on the chemical environment of reaction active centers,and provides the theoretical guidance for controlling the doping distance of heteroatoms to achieve optimal catalytic activity and selectivity.

关键词： distance effect microenvironment heteroatom doping FeN_(4) Sabatier-like relationship structure-activity relationship

Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction of emerging contaminants

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Frontiers of Environmental Science & Engineering 2024年第4期18卷 49-60页

作者： Yuhang Liu Wenxuan Deng Xiaojun Wu Chun Hu Lai Lyu Key Laboratory for Water Quality and Conservation of the Pearl River Delta(Ministry of education) Institute of Environmental Research at Greater BayGuangzhou UniversityGuangzhou 510006China

Effective removal of emerging contaminants(ECs)to minimize their impacts on human health and the natural environment is a global *** the removal of ECs in water,we fabricated a seaweed spherical microsphere catalyst with Cu cation-πstructures by in situ doping of Cu species and ascorbic acid in mesoporous silica(Cu-C-MSNs)via a hydrothermal *** results indicate that bisphenol A(BPA)is substantially degraded within 5 min under natural conditions,with its biological toxicity considerably ***,industrial wastewater could also be effectively purified by Cu-C-MSNs/H_(2)O_(2) *** presence of metal sites and the complexation of ECs via cation-πinteraction andπ-πstacking on the catalyst surface were directly responsible for the polarization distribution of electrons,thus activating H_(2)O_(2) and dissolved oxygen(DO).The removal of contaminants could be attributed primarily to 1)the activation of H_(2)O_(2) into ^(·)OH to attack the contaminants and 2)self-cleavage because of the transfer of electrons from the contaminants to the *** study provides an innovative solution for the effective treatment of ECs and has positive implications for easing global environmental crises.

关键词： Cation-πstructures Polarization electric field Fenton-like process Contaminants cleavage

3D nano-printed geometric phase metasurfaces for generating accelerating beams with complex amplitude manipulation

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Science China(Physics,Mechanics & Astronomy) 2024年第6期67卷 86-95页

作者： Tianchen Tang Saima Kanwal Yongzheng Lu Yuelong Li Shuangbao Wu Lei Chen Ziheng Qian Zhouyu Xie Jing Wen Dawei Zhang research Center of Optical Instrument and System Ministry of Education and Shanghai Key Lab of Modern Optical SystemUniversity of Shanghai for Science and TechnologyShanghai 200093China

Metasurface,a forefront in emerging optical devices,has demonstrated remarkable potential for complex amplitude manipulation of light ***,prevailing approaches face challenges in spatial resolution and complexities associated with integrating dynamic phases,impeding the simplified design and reproducible fabrication of ***,we introduce an innovative approach for complex amplitude modulation within 3D nano-printed geometric phase *** approach enables the generation of self-accelerating beams by encoding amplitude through phase-only manipulation,achieving high spatial ***,this method circumvents the conventional need to adjust the geometric parameters of metasurface unit structures for amplitude manipulation,offering a streamlined and efficient route for design and fabrication *** novel methodology holds promise for expedited and low-cost manufacturing of complex amplitude manipulation metasurfaces.

关键词： metasurface complex amplitude manipulation geometric phase 3D nano-printing Airy beam accelerating parabolic beam

Combining anodic alcohol oxidative coupling for C-C bond formation with cathodic ammonia production

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National Science Review 2024年第5期11卷 217-226页

作者： Leitao Xu Wei Chen Cairong Wang Wenjie Wu Yelin Yao Zhifeng Huang Jingcheng Wu Ming Yang Yandong Wu Dianke Xie Yuqin Zou Shuangyin Wang State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of Education Hunan University

Electrocatalytic oxidation of alcohols using heterogeneous catalysts is a promising aqueous, energy-efficient and environmentally friendly approach, especially for coupling different alcohols to prolong the carbon chain via co-oxidation. Precisely regulating critical steps to tailor electrode materials and electrolyte composition is key to selectively coupling alcohols for targeted synthesis. However, selectively coupling different alcohols remains challenging due to the lack of effective catalyst and electrolyte design promoting specific pathways. Herein, we demonstrate a paired electrolysis strategy for combining anodic oxidative coupling of ethanol（EtOH） and benzyl alcohol（PhCH2OH） to synthesize cinnamaldehyde（CAL） and cathodic ammonia production. The strategies involve:（i） utilizing the salt-out effect to balance selective oxidation and coupling rates;（ii） developing platinum-loaded nickel hydroxide electrocatalysts to accelerate intermediate coupling kinetics;（iii） introducing thermodynamically favorable nitrate reduction at the cathode to improve coupling selectivity by avoiding hydrogenation of products while generating valuable ammonia instead of hydrogen. We achieved 85% coupling selectivity and 278 μmol/h NH3productive rate at 100 m A/cm2with a low energy input（～1.63 V）. The membrane-free, low energy, scalable approach with a wide substrate scope highlights promising applications of this methodology. This work advances heterogeneous electrocatalytic synthesis through rational design principles that integrate anodic oxidative coupling with cathodic nitrate reduction reactions, having synergistic effects on efficiency and selectivity.

关键词： anodic alcohol oxidative coupling C–C bond formation cinnamaldehyde cathodic ammonia production