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Selective Electrochemical Reduction of Nitrogen to Ammonia by Adjusting the Three-Phase Interface

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Research 2019年第1期2019卷 66-77页

作者： Haiyan Wang Yuzhuo chen Ruxue Fan jiadong chen Zhe Wang Shanjun Mao Yong Wang Advanced Materials and Catalysis Group Institute of CatalysisDepartment of ChemistryZhejiang UniversityHangzhou 310028China

The electrochemical nitrogen reduction reaction(NRR)provides a sustainable and alternative avenue to the Haber-Bosch process for ammonia(NH_(3))*** the great efforts made on catalysts and electrolytes,unfortunately,current NRR suffers from low selectivity due to the overwhelming competition with the hydrogen evolution reaction(HER).Here,we present an adjusted three-phase interface to enhance nitrogen(N_(2))coverage on a catalyst surface and achieve a record-high Faradic efficiency(FE)up to 97%in aqueous *** almost entirely suppressed HER process combined with the enhanced NRR activity,benefiting from the efficient three-interface contact line,is responsible for the excellent selectivity toward NH_(3),as evidenced by the theoretical and experimental *** strategy also demonstrates the applicability to other catalysts that feature strong H adsorption ability,to boost the FE for NH_(3) synthesis above 90%and to improve the NRR activity by engineering the catalysts.

关键词： synthesis solution selectivity

Modulating Pd e_(g) orbital occupancy in Pd-Au metallic aerogels for efficient carbon dioxide reduction

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Journal of Energy Chemistry 2023年第12期87卷 98-104,I0004页

作者： Yao chen Juan Wang Tingjie Mao Cun chen Hanjun Li Honggang Huang Hui Fu Feili Lai jiadong chen Nan Zhang Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringInternational Joint Research Laboratory for Nano Energy CompositesJiangnan UniversityWuxi 214122JiangsuChina Key Laboratory of Leather of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035ZhejiangChina Department of Chemistry KU LeuvenCelestijnenlaan 200FLeuven 3001Belgium

The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the ***,we present a new strategy to modulate the e_(g) orbital occupancy of Pd by constructing composition-controllable Pd-Au metallic aerogels(MAs),optimizing the d-band center of Pd to achieve excellent performance for electrochemical carbon dioxide reduction reaction(CO_(2)RR).Specifically,Pd_(1)Au_(2) MAs achieve almost 100% Faraday efficiency(FE) of CO in the range of-0.40 to-0.80 V *** hydrogen electrode(RHE),as well as the long-term stability,being one of the best Pd-based materials for CO_(2)*** X-ray photoelectron spectroscopy(XPS) results and density functional theory(DFT) calculations demonstrate that the introduction of Au modulates the Pd e_(g) orbital occupancy,which significantly weakens *CO adsorption on Pd,reduces the CO_(2)RR energy barrier and consequently improves the electrocatalytic activity and stability for long-term *** work highlights a new strategy for designing efficient electrocatalysts for CO_(2)RR and beyond.

关键词： Pd Carbon dioxide reduction Alloy Aerogels Orbital occupancy

A novel polymer-based nitrocellulose platform for implementing a multiplexed microfluidic paperbased enzyme-linked immunosorbent assay

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Microsystems & Nanoengineering 2022年第3期8卷 199-208页

作者： Dong Lin Bowei Li Longwen Fu Ji Qi Chunlei Xia Yi Zhang jiadong chen Jaebum Choo Lingxin chen CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation Shandong Key Laboratory of Coastal Environmental ProcessesYantai Institute of Coastal Zone ResearchChinese Academy of Sciences264003 YantaiChina School of Pharmacy Binzhou Medical University264003 YantaiChina University of Chinese Academy of Sciences 100049 BeijingChina Center for Ocean Mega-Science Chinese Academy of Sciences266071 QingdaoChina Institute of Analytical Food Safety School of Food Science and TechnologyJiangnan University214122 WuxiChina Department of Chemistry Chung-Ang UniversitySeoul 06974South Korea

Nitrocellose(NC)membranes,as porous paper-like substrates with high protein-binding capabilties,are very popular in the field of point-of-care ***,generating robust hydrophobic structures in NC membranes to fabricate microfluidic paper-based analytical devices(μPADs)remains a great *** present,the main method relies on an expensive wax printer In addition,NC membranes very easy to adhere during the printing process due to electrostatic ***,we developed a facile,fast and low-cost strategy to fabricateμPADs in NC membranes by screen-printing polyurethane acrylate(PUA)as a barrier material for defning flow channels and reaction ***,hydrophobic barriers based on UV-curable PUA can resist various surfactant solutions and organic solvents that are generally used in immunoassays and biochemical *** validate the feasibility of this PUA-based NC membrane for immunoassays in point-of-care testing(POCT),we further designed and assembled a rotational paperbased analytical device for implementing a multiplexed enzyme-linked immunosorbent assay(ELISA)in a simple *** the proposed device under the optimal conditions,alpha fetoprotein(AFP)and carcinoembryonic antigen(CEA)could be identified,with limits of detection of 136 pg/mL and 174 pg/mL,respectively,which are below the threshold values of these two cancer biomarkers for clinical *** believe that this reliable device provides a promising plaform for the diagnosis of disease based on ELISA or other related bioassays in limited setings or remote regions.

关键词： diagnosis printing cellulose

Lattice-distorted Pt wrinkled nanoparticles for highly effective hydrogen electrocatalysis

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Nano Research 2024年第5期17卷 3819-3826页

作者： Xue Li Xiang Han Zhenrui Yang Shun Wang Yun Yang Juan Wang jiadong chen Zhongwei chen Huile Jin Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Institute of New Materials and Industry Technology College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterlooOntario N2L 3G1Canada

Modulating Pt surfaces through the introduction of lattice distortion emerges as immensely effective strategy that enhances the kinetics of alkaline hydrogen evolution and oxidation *** this study,we fabricated lattice-distorted Pt wrinkled nanoparticles(LD-Pt WNPs)for efficient hydrogen *** LD-Pt WNPs not only outperform the Pt/C benchmark in hydrogen oxidation reaction,achieving an excellent mass-specific current of 968.5 mA·mg_(Pt)^(-1)(9 times that of Pt/C),but also demonstrate outstanding hydrogen evolution reaction activity with a small overpotential of 58.0 *** experiments and density functional theory calculations reveal that lattice defects introduce an abundance of unsaturated coordination atoms while modifying the d-band center of *** dual effect optimizes the binding strength of crucial H and OH intermediates,leading to a significant reduction in the energy barrier of the reaction bottleneck,commonly known as the Volmer *** work unveils a fresh viewpoint on projecting and developing high efficiency electrocatalysts through defect engineering.

关键词： distortion nanoparticle hydrogen evolution reaction defect engineering hydrogen oxidation reaction

Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano Research 2024年第5期17卷 3801-3809页

作者： Yan chen Zhenrui Yang Juan Wang Yun Yang Xuedong He Yang Wang jiadong chen Yaqing Guo Xin Wang Shun Wang Huile Jin Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang Engineering Research Center for Electrochemical Energy Materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective ***,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),*** addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air *** experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and *** functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of *** electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster *** study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

Intercalation-Assisted Co-Doped MoS_(2) Nanoflowers for an Efficient Hydrogen Evolution Reaction

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Precision Chemistry 2023年第8期1卷 497-506页

作者： Minkai Qin Menghui Qi Ruxue Fan jiadong chen Xiaoyun Shi Binbin Lin Lingling Xi Yong Wang Advanced Materials and Catalysis Group Center of Chemistry for Frontier TechnologiesState Key Laboratory of Clean Energy UtilizationInstitute of CatalysisDepartment of ChemistryZhejiang UniversityHangzhou 310028P.R.China College of Chemistry and Molecular Engineering Zhengzhou UniversityZhengzhou 450001P.R.China

2D transition metal disulfides have emerged as promising Pt-alternative electrocatalysts for hydrogen ***,the sluggish water dissociation kinetics and limited active sites hinder their performance in alkaline ***,we propose a two-step hydrothermal method to synthesize K intercalation-assisted Codoped MoS_(2) *** nanoflowers exhibit an overpotential of only 67 mV at a current density of 10 mA cm^(-2),which exceeds that of pristine MoS_(2)(143 mV).We demonstrated that the intercalation of K enlarges the interlayer spacing of MoS_(2) nanosheets and facilitates the doping of *** incorporation of Co effectively improves the surface charge transfer efficiency of MoS_(2) and accelerates water splitting with an energy barrier of 0.12 *** work offers an approach to activate the inert MoS_(2) basal plane by chemical intercalation and atomic doping *** can be extended to develop other functional materials beyond water splitting.

关键词： molybdenum disulfides heteroatomic doping chemical intercalation hydrogen evolution reaction hydrophilicity

Phosphorylated TDP-43 Staging of Primary Age-Related Tauopathy

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Neuroscience Bulletin 2019年第2期35卷 183-192页

作者： Xiaoling Zhang Bing Sun Xing Wang Hui Lu Fangjie Shao Annemieke J.M.Rozemuller Huazheng Liang Chong Liu jiadong chen Manli Huang Keqing Zhu China Brain Bank and Department of Neurology in Second Affiliated Hospital Key Laboratory of Medical Neurobiology of Zhejiang ProvinceDepartment of NeurobiologyZhejiang University School of Medicine Department of Pathology Zhejiang University School of Medicine Department of Pathology Amsterdam NeuroscienceVU University Medical Center Brain Structure and Function Group Neuroscience Research Australia Department of Psychiatry First Affiliated HospitalZhejiang University School of Medicine

Primary age-related tauopathy(PART) is characterized by tau neurofibrillary tangles(NFTs) in the absence of amyloid plaque pathology. In the present study,we analyzed the distribution patterns of phosphorylated43-kDa TAR DNA-binding protein(pTDP-43) in the brains of patients with PART. Immunohistochemistry and immunofluorescence double-labeling in multiple brain regions was performed on brain tissues from PART,Alzheimer's disease(AD), and aging control cases. We examined the regional distribution patterns of pTDP-43 intraneuronal inclusions in PART with Braak NFT stages[ 0 and B IV, and a Thal phase of 0(no beta-amyloid present). We found four stages which indicated potentially sequential dissemination of pTDP-43 in PART. Stage I was characterized by the presence of pTDP-43 lesions in the amygdala, stage II by such lesions in the hippocampus,stage III by spread of pTDP-43 to the neocortex, and stage IV by pTDP-43 lesions in the putamen, pallidum, and insular cortex. In general, the distribution pattern of pTDP-43 pathology in PART cases was similar to the early TDP-43 stages reported in AD, but tended to be more restricted to the limbic system. However, there were some differences in the distribution patterns of pTDP-43 between PART and AD, especially in the dentate gyrus of the hippocampus. Positive correlations were found in PART between the Braak NFT stage and the pTDP-43 stage and density.

关键词： TDP-43 Primary age-related tauopathy Alzheimer's disease Neurofibrillary tangle Hippocampus

Somatostatin-Positive Neurons in the Rostral Zona Incerta Modulate Innate Fear-Induced Defensive Response in Mice

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Neuroscience Bulletin 2023年第2期39卷 245-260页

作者： Shan Lin Meng-Yue Zhu Meng-Yu Tang Mi Wang Xiao-Dan Yu Yi Zhu Shi-Ze Xie Dan Yang jiadong chen Xiao-Ming Li Department of Neurobiology and Department of Neurology of the Second Afliated Hospital Zhejiang University School of MedicineHangzhou 310058China NHC and CAMS Key Laboratory of Medical Neurobiology MOE Frontier Science Center for Brain Research and Brain-Machine IntegrationSchool of Brain Science and Brian MedicineZhejiang UniversityHangzhou 310058China Center for Brain Science and Brain-Inspired Intelligence Research Units for Emotion and Emotion DisordersChinese Academy of Medical SciencesChina/Guangdong-Hong Kong-Macao Greater Bay AreaJoint Institute for Genetics and Genome Medicine between Zhejiang University and the University of TorontoHangzhou 310058China

Defensive behaviors induced by innate fear or Pavlovian fear conditioning are crucial for animals to avoid threats and ensure *** zona incerta(ZI)has been demonstrated to play important roles in fear learning and fear memory,as well as modulating auditory-induced innate defensive ***,whether the neuronal subtypes in the ZI and specific circuits can mediate the innate fear response is largely ***,we found that somatostatin(SST)-positive neurons in the rostral ZI of mice were activated by a visual innate fear *** inhibition of SST-positive neurons in the rostral ZI resulted in reduced flight responses to an overhead looming *** activation of SST-positive neurons in the rostral ZI induced fear-like defensive behavior including increased immobility and *** addition,we demonstrated that manipulation of the GABAergic projections from SST-positive neurons in the rostral ZI to the downstream nucleus reuniens(Re)mediated fear-like defensive *** trans-synaptic tracing also revealed looming stimulus-activated neurons in the superior colliculus(SC)that projected to the Re-projecting SST-positive neurons in the rostral ZI(SC-ZIrSST-Re pathway).Together,our study elucidates the function of SST-positive neurons in the rostral ZI and the SC-ZIrSST-Re tri-synaptic circuit in mediating the innate fear response.

关键词： Innate fear Zona incerta Somatostatinpositive neurons Looming stimulus Defensive behavior

Pathological Networks Involving Dysmorphic Neurons in Type ⅡFocal Cortical Dysplasia

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Neuroscience Bulletin 2022年第9期38卷 1007-1024页

作者： Yijie Shao Qianqian Ge Jiachao Yang Mi Wang Yu Zhou Jin-Xin Guo Mengyue Zhu Jiachen Shi Yiqi Hu Li Shen Zhong chen Xiao-Ming Li Jun-Ming Zhu Jianmin Zhang Shumin Duan jiadong chen Center for Neuroscience and Department of Neurosurgery of the Second Affiliated Hospital NHC and CAMS Key Laboratory of Medical NeurobiologyMOE Frontier Science Center for Brain Research and Brain-Machine IntegrationSchool of Brain Science and Brain MedicineZhejiang University School of MedicineHangzhou310058China Department of Neurosurgery of the Second Affiliated Hospital Zhejiang University School of MedicineHangzhou310009China The MOE Key Laboratory of Biosystems Homeostasis&Protection and Zhejiang Provincial Key Laboratory for Cancer Molecular Cell Biology Life Sciences InstituteZhejiang UniversityHangzhou310058China Department of Orthopedic Surgery School of Medicinethe Second Affiliated HospitalZhejiang UniversityHangzhou310009China Hangzhou Innovation Center Zhejiang UniversityHangzhou310058China Institute of Pharmacology&Toxicology NHC and CAMS Key Laboratory of Medical NeurobiologyCollege of Pharmaceutical SciencesSchool of Basic Medical SciencesZhejiang UniversityHangzhou310058China Key Laboratory of Neuropharmacology and Translational Medicine of Zhejiang Province College of Pharmaceutical SciencesZhejiang Chinese Medical UniversityHangzhou310058China Center for Neuroscience and Department of Neurology of the Second Affiliated Hospital Zhejiang University School of MedicineHangzhou310058China NHC and CAMS Key Laboratory of Medical Neurobiology Center for Brain Science and Brain-Inspired IntelligenceJoint Institute for Genetics and Genome Medicine betweenGuangdong Hong Kong Macao Greater Bay AreaZhejiang University and the University of TorontoZhejiang University School of MedicineHangzhou310058China

Focal cortical dysplasia(FCD)is one of the most common causes of drug-resistant *** neurons are the major histopathological feature of typeⅡFCD,but their role in seizure genesis in FCD is *** we performed whole-cell patch-clamp recording and morphological reconstruction of cortical principal neurons in postsurgical brain tissue from drug-resistant epilepsy *** analyses revealed distinct morphological and electrophysiological characteristics of the upper layer dysmorphic neurons in typeⅡFCD,including an enlarged soma,aberrant dendritic arbors,increased current injection for rheobase action potential firing,and reduced action potential firing ***,the upper layer dysmorphic neurons received decreased glutamatergic and increased GABAergic synaptic inputs that were coupled with upregulation of the Na^(+)-K^(+)-Cl^(−)*** addition,we found a depolarizing shift of the GABA reversal potential in the CamKⅡ-cre::PTENflox/flox mouse model of drug-resistant epilepsy,suggesting that enhanced GABAergic inputs might depolarize dysmorphic ***,imbalance of synaptic excitation and inhibition of dysmorphic neurons may contribute to seizure genesis in typeⅡFCD.

关键词： Focal cortical dysplasia Dysmorphic neuron Whole-cell patch-clamp recording Morphological reconstruction Excitation-inhibition balance