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| 1 | Nitrogen reduction reaction on small iron clusters supported by N-doped graphene:A theoretical study of the atomically precise active-site mechanism显示文摘Nonprecious metal catalysts are known of significance for electrochemical N2 reduction reaction(NRR)of which the mechanism has been illustrated by ongoing investigations of single atom catalysis.However,it remains challenging to fully understand the size-dependent synergistic effect of active sites inherited in substantial nanocatalysts.In this work,four types of small iron clusters Fen(n=1–4)supported on nitrogen-doped graphene sheets are constructed to figure out the size dependence and synergistic effect of active sites for NRR catalytic activities.It is revealed that Fe3 and Fe4 clusters on N4G supports exhibit higher NRR activity than single-iron atom and iron dimer clusters,showing lowered limiting potential and restricted hydrogen evolution reaction(HER)which is a competitive reaction channel.In particular,the Fe4-N4G displays outstanding NRR performance for“side-on”adsorption of N2 with a small limiting potential(−0.45 V).Besides the specific structure and strong interface interaction within the Fe4-N4G itself,the high NRR activity is associated with the unique bonding/antibonding orbital interactions of N-N and N-Fe for the adsorptive N2 and NNH intermediates,as well as relatively large charge transfer between N2 and the cluster Fe4-N4G. | Chaonan Cui Hongchao Zhang Zhixun Luo | 2020 | Nano Research2020,13,8: | 4 |
| 2 | Nitrogen-carbon layer coated nickel nanoparticles for efficient electrocatalytic reduction of carbon dioxide显示文摘The application of nickel in electrocatalytic reduction of CO2 has been largely restricted by side reaction (hydrogen evolution reaction) and catalyst poisoning.Here we report a new strategy to improve the electrocatalytic performance of nickel for CO2 reduction by employing a nitrogen-carbon layer for nickel nanoparticles.Such a nickel electrocatalyst exhibits high Faradaic efficiency 97.5% at relatively low potential of-0.61 V for the conversion of CO2 to CO.Density functional theory calculation reveals that it is thermodynamically accomplishable for the reduction product CO to be removed from the catalyst surface,thus avoiding catalyst poisoning.Also,the catalyst renders hydrogen evolution reaction to be suppressed and hence reasonably improves catalytic performance. | Dongxing Tan Chaonan Cui Jinbiao Shi Zhixun Luo Bingxing Zhang Xiuniang Tan Buxing Han Lirong Zheng Jing Zhang Jianling Zhang | 2019 | Nano Research2019,12,5: | 3 |
| 3 | A facile method to synthesize water-soluble Pd8 nanoclusters unraveling the catalytic mechanism of p-nitrophenol to p-aminophenol显示文摘Hydroge nation of p-n itrophe nol(PNP)towards the con versi on to p-ami nophe no I(PAP)by metal catalysis is known as a simple and I eco-frie ndly tech nique for the production of corresp on ding in dustrial and pharmaceutical in termediates.While continu ous efforts are paid for§more sustainable and greener procedures by using transition metal catalysts,atomic-precise reaction mechanism for the PNP-to-PAP is still illusive to be fully un derstood.Utilizi ng a dry-wet com bined strategy,here we have syn thesized water-soluble Pd8 nano clusters(NCs)with mercaptosuccinic acid(H2SMA)as the ligand,and the Pd8 NCs found high catalytic performance for the conversion of PNP-to-PAP,as identified by the electrospray ionization mass spectrometer(ESI-MS)measurement.The gradual changes over time of ultraviolet-visible(UV-vis)spectra of PNP really display the catalytic reduction by NaBH4 in presence of Pd8 NCs.Further,in-depth charge transfer interactions between PNP and the Pd8 clusters at the proton-rich conditions are investigated by natural bond orbital(NBO)analysis and electron density differenee(EDD)analysis.The exothermic and kinetic-favorable reaction pathways are addressed,based on successive PNP hydrogenation and H2O removal processes,clarifying the reaction mechanism of Pd catalysts.It is worth noting that this solid-state synthetic route for such Pd8 clusters enables gram-scale quantity of production in likely practical use. | Pan An Rajini Anumula Chaonan Cui Yang Liu Fei Zhan Ye Tao Zhixun Luo | 2019 | Nano Research2019,12,10: | 2 |
| 4 | A distinct D1-MSN subpopulation down-regulates dopamine to promote negative emotional state显示文摘Dopamine(DA)level in the nucleus accumbens(NAc)is critical for reward and aversion encoding.DA released from the ventral mesencephalon(VM)DAergic neurons increases the excitability of VM-projecting D1-dopamine receptor-expressing medium spiny neurons(D1-MSNs)in the NAc to enhance DA release and augment rewards.However,how such a DA positive feedback loop is regulated to maintain DA homeostasis and reward-aversion balance remains elusive.Here we report that the ventral pallidum(VP)projection of NAc D1-MSNs(D1^(NAc-VP))is inhibited by rewarding stimuli and activated by aversive stimuli.In contrast to the VM projection of D1-MSN(D1^(NAc-VM)),activation of D1^(NAc-VP) projection induces aversion,but not reward.D1^(NAc-VP) MSNs are distinct from the D1^(NAc-VM) MSNs,which exhibit conventional functions of D1-MSNs.Activation of D1^(NAc-VP) projection stimulates VM GABAergic transmission,inhibits VM DAergic neurons,and reduces DA release into the NAc.Thus,D1^(NAc-VP) and D1^(NAc-VM) MSNs cooperatively control NAc dopamine balance and reward-aversion states. | Zhiyuan Liu Qiumin Le Yanbo Lv Xi Chen Jian Cui Yiming Zhou Deqin Cheng Chaonan Ma Xiujuan Su Lei Xiao Ruyi Yang Jiayi Zhang Lan Ma Xing Liu | 2022 | Cell Research2022,32,2: | 2 |
| 5 | In-situ generation and global property profiling of metal nanoclusters by ultraviolet laser dissociation-mass spectrometry显示文摘Metal nanoclusters are promising nanomaterials with unique properties, but only a few ones with specific numbers of metal atoms can be obtained and studied up to now. In this study, we establish a new paradigm of in-situ generation and global study of metal nanoclusters with different sizes, constitutions, and charge states, including both accurate constitution characterization and global activity profiling. The complex mixtures of metal nanoclusters are produced by employing single-pulsed 193-nm laser dissociation of monolayer-protected cluster(MPC) precursors within a high-resolution mass spectrometry(HRMS). More than400 types of bare gold nanoclusters including novel multiply charged(2+ and 3+), S-/P-doped, and silver alloy ones can be efficiently generated and accurately characterized. A distinct size(1 to 142 atoms)-and charge(1+ to 3+)-hierarchy reactivity is clearly observed for the first time. This global cluster study might greatly promote the developments and applications of novel metal nanoclusters. | Zheyi Liu Zhaoxian Qin Chaonan Cui Zhixun Luo Bing Yang You Jiang Can Lai Zhipeng Wang Xiaolei Wang Xiang Fang Gao Li Fangjun Wang Chunlei Xiao Xueming Yang | 2022 | Science China Chemistry2022,65,6: | 2 |
| 6 | Small gold clusters catalyzing oxidant-free dehydrogenation of glycerol initiated by methene hydrogen atom transfer显示文摘Developing oxygen-free methodology for the conversion of alcohols to carbonyls is essentially important because it suppresses the over-oxidation of alcohols to carboxylic acids and enables the production of energetic hydrogen.Here we report a finding of feasible oxidant-free dehydrogenation of glycerol over chemically-pure Au clusters synthesized by a green chemistry method named as laser ablation in liquid(LAL).As results,glycerol is dehydrogenated to form glyceraldehyde which undergoes subsequent dehydrogenation to hydroxymethyl glyoxal.For this,reaction dynamics calculations find interesting dehydrogenation reaction pathways with a low-energy barrier of transition state initiated by hydrogen atom transfer from methene,which differs from the general reaction mechanism based on hydroxyl.Furthermore,it is interesting that the presence of additionalààOH group molecules especially H2O can effectively lower the energy barrier in the activation of the OààH and CààH bonds in glycerol.This principle is also applicable to the oxidant-free dehydrogenation of methanol and ethanol,helping to fully understand the catalytic mechanism of alcohols conversion chemistry. | Anthony M.S.Pembere Chaonan Cui Haiming Wu Zhixun Luo | 2019 | Chinese Chemical Letters2019,30,5: | 1 |
| 7 | DHD4,a CONSTANS-like family transcription factor,delays heading date by affecting the formation of the FAC complex in rice显示文摘Heading date(or flowering time)is one of the most important agronomic traits in rice,influencing its regional adaptability and crop yield.Many major-effect genes for rice heading date have been identified,but in practice they are difficult to be used for rice molecular breeding because of their dramatic effects on heading date.Genes with minor effects on heading date,which are more desirable for fine-tuning flowering time without significant yield penalty,were seldom reported.In this study,we identified a new minor-effect heading date repressor,Delayed Heading Date 4(DHD4).The dhd4 mutant shows a slightly earlier flowering phenotype without a notable yield penalty compared with wild-type plants under natural long-day conditions.DHD4 encodes a CONSTANS-like transcription factor localized in the nucleus.Molecular,biochemical,and genetic assays show that DHD4 can compete with 14-3-3 to interact with OsFD1,thus affecting the formation of the Hd3a-14-3-3-OsFD1 triprotein FAC complex,resulting in reduced expression of OsMADS14 and OsMADS15,and ultimately delaying flowering.Taken together,these results shed new light on the regulation of flowering time in rice and provide a promising target for fine-tuning flowering time to improve the regional adaptability of rice. | Maohong Cai Shanshan Zhu Mingming Wu Xiaoming Zheng Jiachang Wang Liang Zhou Tianhui Zheng Song Cui Shirong Zhou Chaonan Li Huan Zhang Juntao Chai Xinyue Zhang Xin Jin Zhijun Cheng Xin Zhang Cailin Lei Yulong Ren Qibing Lin Xiuping Guo Lei Zhao Jie Wang Zhichao Zhao Ling Jiang Haiyang Wang Jianmin Wan | 2021 | Molecular Plant2021,14,2: | 1 |
| 8 | Plasma-Assisted Dinitrogen Activation via Dual Platinum Cluster Catalysis:A Strategy for Ammonia Synthesis under Mild Conditions显示文摘The activation and reduction of N_(2)to produce ammonia under mild conditions is of great interest,but challenges remain.Here,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1–4)clusters and convenient plasma assistance.The reactivity of Pt3+is found to be substantially higher than that of other clusters,and the formed Pt3N7+shows prominent mass abundance among the odd-nitrogen products.We illustrate that a chain reaction path within dual cluster cooperation,especially via a“3+2”mode,is beneficial to N≡N triple bond dissociation,embodying efficient synergistic catalysis.A key intermediate containing a bridged N_(2)of binding with two Pt clusters facilitates N_(2)activation with significantly enhanced interactions between the d orbitals of Pt and the antibondingπ*-orbitals of N_(2).Furthermore,by reacting the Pt_(n)N_(m)+clusters with H_(2),we observed hydrogenation products of both evenand odd-hydrogen species,indicative of ammonia release.The in situ synthesized platinum nitride clusters,typically Pt_(3)N_(7)+,induce a highly active N site for hydrogen anchoring,enabling a cost-effective hydrotreating process for ammonia synthesis. | Chaonan Cui Yuhan Jia Hanyu Zhang Lijun Geng Zhixun Luo | 2023 | CCS Chemistry2023,5,3: | 0 |
| 9 | Translational oncology toward benefiting cancer patients:the Sun Yat-sen University Cancer Center experience显示文摘Cancer is a leading cause of death in China with an estimation of nearly 2 million deaths every year(Chen and Fu,2011b).Matter of a public health importance in China and worldwide,the scientific community is still facing | Mathilde Guerin Chaonan Qian Qian Zhong Qian Cui Yunmiao Guo Jinxin Bei Jianyong Shao Xiaofeng Zhu Wenlin Huang Jiangxue Wu Ranyi Liu Qiang Liu Jing Wang Weihua Jia Xiaohui Zheng Yixin Zeng | 2016 | Science China(Life Sciences)2016,59,10: | 0 |
| 10 | A DFT study of CO_2 electrochemical reduction on Pb(211) and Sn(112)显示文摘Electrochemical reduction of CO2 has the benefit of turning greenhouse gas emissions into useful resources. We performed a comparative study of the electrochemical reduction of CO2 on stepped Pb(211) and Sn(112) surfaces based on the results of density functional theory slab calculations. We mapped out the potential energy profiles for electrochemical reduction of CO2 to formate and other possible products on both surfaces. Our results show that the first step is the formation of the adsorbed formate(HCOO*) species through an Eley-Rideal mechanism. The formate species can be reduced to HCOO- through a oneelectron reduction in basic solution, which produces formic acid as the predominant product. The respective potentials of forming HCOO* are predicted to be -0.72 and -0.58 V on Pb and Sn. Higher overpotentials make other reaction pathways accessible, leading to different products. On Sn(112), CO and CH4 can be generated at -0.65 V following formate formation. In contrast, the limiting potential to access alternative reaction channels on Pb(211) is -1.33 V, significantly higher than that of Sn. | Chaonan Cui Hua Wang Xinli Zhu Jinyu Han Qingfeng Ge | 2015 | Science China Chemistry2015,58,4: | 0 |
| 11 | Hepatic Zbtb18 (Zinc Finger and BTB Domain Containing 18) alleviates hepatic steatohepatitis via FXR (Farnesoid X Receptor)显示文摘A lasting imbalance between fatty acid synthesis and consumption leads to non-alcoholic fatty liver disease(NAFLD),coupled with hepatitis and insulin resistance.Yet the details of the underlying mechanisms are not fully understood.Here,we unraveled that the expression of the transcription factor Zbtb18 is markedly decreased in the livers of both patients and murine models of NAFLD.Hepatic Zbtb18 knockout promoted NAFLD features like impaired energy expenditure and fatty acid oxidation(FAO),and induced insulin resistance.Conversely,hepatic Zbtb18 overexpression alleviated hepato-steatosis,insulin resistance,and hyperglycemia in mice fed on a high-fat diet(HFD)or in diabetic mice.Notably,in vitro and in vivo mechanistic studies revealed that Zbtb18 transcriptional activation of Farnesoid X receptor(FXR)mediated FAO and Clathrin Heavy Chain(CLTC)protein hinders NLRP3 inflammasome activity.This key mechanism by which hepatocyte’s Zbtb18 expression alleviates NAFLD and consequent liver fibrosis was further verified by FXR’s deletion and forced expression in mice and cultured mouse primary hepatocytes(MPHs).Moreover,CLTC deletion significantly abrogated the hepatic Zbtb18 overexpression-driven inhibition of NLRP3 inflammasome activity in macrophages.Altogether,Zbtb18 transcriptionally activates the FXR-mediated FAO and CLTC expression,which inhibits NLRP3 inflammasome’s activity alleviating inflammatory stress and insulin resistance,representing an attractive remedy for hepatic steatosis and fibrosis. | Lei Zhang Jiabing Chen Xiaoying Yang Chuangpeng Shen Jiawen Huang Dong Zhang Naihua Liu Chaonan Liu Yadi Zhong Yingjian Chen Kaijia Tang Jingyi Guo Tianqi Cui Siwei Duan Jiayu Li Shangyi Huang Huafeng Pan Huabing Zhang Xiaoqiang Tang Yongsheng Chang Yong Gao | 2024 | Signal Transduction and Targeted Therapy2024,9,2: | 0 |
| 12 | Enhanced Catalysis of Pt_(3) Clusters Supported on Graphene for N–H Bond Dissociation显示文摘We report an in-depth study of catalytic N–H bond dissociation with typical platinum clusters on gra-phene supports.Among all the pristine graphene-and defective graphene-supported Pt clusters of different sizes that were studied,the Pt_(3)/G cluster possesses the highest reactivity and lowest activa-tion barriers for each step of N–H dissociation in the decomposition of ammonia. | Chaonan Cui Zhixun Luo Jiannian Yao | 2019 | CCS Chemistry2019,1,2: | 0 |
| 13 | Co_(13)O_(8)—metalloxocubes:a new class of perovskite-like neutral clusters with cubic aromaticity显示文摘Exploring stable clusters to understand structural evolution from atoms to macroscopic matter and to construct new materials is interesting yet challenging in chemistry.Utilizing our newly developed deep-ultraviolet laser ionization mass spectrometry technique,here we observe the reactions of neutral cobalt clusters with oxygen and find a very stable cluster species of Co13O8 that dominates the mass distribution in the presence of a large flow rate of oxygen gas.The results of global-minimum structural search reveal a unique cubic structure and distinctive stability of the neutral Co13O8 cluster that forms a new class of metal oxides that we named as‘metalloxocubes’.Thermodynamics and kinetics calculations illustrate the structural evolution from icosahedral Co13 to the metalloxocube Co13O8 with decreased energy,enhanced stability and aromaticity.This class of neutral oxygen-passivated metal clusters may be an ideal candidate for genetic materials because of the cubic nature of the building blocks and the stability due to cubic aromaticity. | Lijun Geng Mouyi Weng Cong-Qiao Xu Hanyu Zhang Chaonan Cui Haiming Wu Xin Chen Mingyu Hu Hai Lin Zhen-Dong Sun Xi Wang Han-Shi Hu Jun Li Jiaxin Zheng Zhixun Luo Feng Pan Jiannian Yao | 2021 | National Science Review2021,8,1: | 0 |
| 14 | Characteristics of dissolved sugars in the Southern Yap Trench from sea surface to hadal zone显示文摘2,4,6-Tripyridine-s-triazine(TPTZ)spectrophotometric method was applied to determine the concentrations of dissolved monosaccharides(MCHO),polysaccharides(PCHO),and total carbohydrate(TCHO)in seawater samples collected from sea surface to hadal zone and sediment-seawater interface of the Southern Yap Trench in the Western Pacific Ocean.Results show that the concentrations of MCHO,PCHO,and TCHO ranged from 6.3 to 22.3μmol C/L,1.1 to 25.4μmol C/L,and 12.1 to 44.9μmol C/L,respectively,from the euphotic layer to the hadal zone of the trench.At different sampling stations,the concentrations of MCHO,PCHO,and TCHO in the seawater showed complex vertical variation characteristics,but the overall variation trends were decreasing with water depth.In the Southern Yap Trench,the maximum concentration of MCHO in the seawater appeared in the euphotic layer,and the minimum in the hadal zone.The maximum concentration of PCHO appeared in the euphotic layer,and the minimum in the bathypelagic layer.The water layer where the maxima and minima of the average concentration of TCHO appeared was consistent with that of PCHO.PCHO was the major component of TCHO in the seawater of the Southern Yap Trench.In the seawater from the sediment-seawater interface,the concentrations of MCHO,PCHO,and TCHO ranged from 8.4 to 10.6μmol C/L,3.8 to 5.8μmol C/L,and 12.2 to 15.2μmol C/L,respectively,and MCHO was the major component of TCHO.The key factors affecting the concentration and existing forms of dissolved sugars in the seawater of the Southern Yap Trench included photosynthesis,respiration,polysaccharide hydrolysis,adsorption and desorption of particulate matter,trench“funnel effect”,deep ocean currents,sediment resuspension,and etc.This study provided fundamental data about labile organic matter in abyss and hadal zone of marine environment,which is significant for further understanding of deep-sea organic carbon cycle. | Dong CUI Chengjun SUN Chaonan GUO Wei CAO Fenghua JIANG Haibing DING | 2023 | Journal of Oceanology and Limnology2023,41,6: | 0 |