Zhixuan Lu - Academia.edu (original) (raw)

Papers by Zhixuan Lu

Research paper thumbnail of Boosting CO2 Hydrogenation to Formate over Edge‐Sulfur Vacancies of Molybdenum Disulfide

Angewandte Chemie International Edition

Synthesis of formate from hydrogenation of carbon dioxide (CO2) is an atom‐economic reaction but ... more Synthesis of formate from hydrogenation of carbon dioxide (CO2) is an atom‐economic reaction but is confronted with challenges in developing high‐performance non‐precious metal catalysts for application of the process. Herein, we report a highly durable edge‐rich molybdenum disulfide (MoS2) catalyst for CO2 hydrogenation to formate at 200 °C, which delivers a high selectivity of over 99 % with a superior turnover frequency of 780.7 h−1 surpassing those of previously reported non‐precious metal catalysts. Multiple experimental characterization techniques combined with theoretical calculations reveal that sulfur vacancies at MoS2 edges are the active sites and the selective production of formate is enabled via a completely new water‐mediated hydrogenation mechanism, in which surface OH* and H* species in dynamic equilibrium with water serve as moderate hydrogenating agents for CO2 with residual O* reduced by hydrogen. This study provides a new route for developing low‐cost high‐perfor...

Research paper thumbnail of In-situ Raman spectroscopic insight into charge delocalization-improved electrical conductivity in metal–cyanide frameworks

Nanoscale

Raman spectroscopy reveals that the enhancement mechanism of electrical conductivity in Prussian ... more Raman spectroscopy reveals that the enhancement mechanism of electrical conductivity in Prussian Blue induced by K ions is charge delocalization.

Research paper thumbnail of Accelerated interfacial proton transfer for promoting electrocatalytic activity

Chemical Science

Adsorbing 4MPy on Pt surface promotes proton transfer at the interfacial layer, maintaining an op... more Adsorbing 4MPy on Pt surface promotes proton transfer at the interfacial layer, maintaining an optimal interfacial pH and promotes electrocatalytic reactions involving proton-coupled electron transfer (PCET) processes.

Research paper thumbnail of A new type of sealed rechargeable lithium–lithium oxide battery based on reversible LiO2/Li2O2 interconversion

Journal of Materials Chemistry A

A new type of sealed battery via the interconversion of LiO2/Li2O2 was developed on the basis of ... more A new type of sealed battery via the interconversion of LiO2/Li2O2 was developed on the basis of the stabilization of LiO2 on the OR-rGO cathode, and a long life of 700 cycles was achieved.

Research paper thumbnail of Operando Electrochemical Xray Diffraction and Raman Spectroscopic Studies Revealing the Alkali-Metal Ion Intercalation Mechanism in Prussian Blue Analogues

Prussian blue analogues are promising cathode material candidates for aqueous rechargeable metal-... more Prussian blue analogues are promising cathode material candidates for aqueous rechargeable metal-ion batteries. Although great efforts have been made on developing materials, there are still rare reports on optimizing cell performance from mechanistic understanding and studies. Here we unveil the alkali-metal-ion intercalation mechanism in Berlin green with a home-built spectroelectrochemical cell for operando X-ray Diffraction (XRD) and Raman spectroscopies, which allows us to obtain the correlated local structure, crystal structure, redox activity, and potential profiles during the charging and discharging processes. We found that the intercalation of Na+ follows a solid solution mechanism leading to a high capacity, and the intercalation of K+ follows a two-phase transition mechanism showing a high voltage. With this understanding, we propose a new strategy using a Na+/K+ hybrid cation electrolyte to realize both high voltage and energy density. This study offers a unique insight for improving the cell performance from the understanding of the reaction mechanism.

Research paper thumbnail of Photoinduced Charge Transfer from a Semiconductor to a Metal Probed at the Single-Nanoparticle Level

Research paper thumbnail of Sensitive and simultaneous surface plasmon resonance detection of free and p53-bound MDM2 proteins from human sarcomas

The Analyst, 2018

Sensitive SPR determination of free and p53-bound MDM2 proteins from sarcoma tissue extracts was ... more Sensitive SPR determination of free and p53-bound MDM2 proteins from sarcoma tissue extracts was carried out in fluidic channels covered with the consensus ds-DNA/p53 conjugate and the consensus ds-DNA, respectively.

Research paper thumbnail of Multiplexed Electrochemical Detection of MiRNAs from Sera of Glioma Patients at Different Stages via the Novel Conjugates of Conducting Magnetic Microbeads and Diblock Oligonucleotide-Modified Gold Nanoparticles

Analytical Chemistry, 2017

MicroRNAs (miRNAs) serve as diagnostic and prognostic biomarkers for a wide variety of cancers. V... more MicroRNAs (miRNAs) serve as diagnostic and prognostic biomarkers for a wide variety of cancers. Via the novel conjugates of gold nanoparticle-coated magnetic microbeads (AuNP-MMBs) and the diblock oligonucleotide (ODN)-modified AuNPs, multiplexed electrochemical assay of miRNAs was performed. The hybridization to target miRNAs leads to the conformational change of the hairpin-structured ODN probes, and the attachment of the diblock ODN-modified AuNPs was achieved. By examining the oxidation peak currents of methylene blue (MB) and ferrocene (Fc) moieties residing on the diblock ODNs, simultaneous quantification of miRNA-182 and miRNA-381 was conducted. The detection signals were significantly enhanced due to the numerous MB and Fc tags on the AuNPs. The proposed assay was highly selective for discriminating miRNAs with similar sequences and detection limits of 0.20 fM and 0.12 fM for miRNA-182 and miRNA-381, respectively, were achieved. The feasibility of the method for sensitive determination of miRNA-182 and miRNA-381 from serum samples of glioma patients at different stages was demonstrated. The sensing protocol thus holds great potential for early diagnosis and treatment of cancer patients.

Research paper thumbnail of In Situ Imaging of Live-Cell Extracellular pH during Cell Apoptosis with Surface-Enhanced Raman Spectroscopy

Analytical Chemistry, 2018

Extracellular pH (pHe) is an important regulating factor that determines many cellular processes,... more Extracellular pH (pHe) is an important regulating factor that determines many cellular processes, including proliferation, differentiation, and apoptosis. In our previous work, we developed 4-MPy (4-mercaptopyridine) modified Au nanoparticles as intracellular pH sensors based on surface-enhanced Raman spectroscopy (SERS). We herein modified Au nanoparticles-assembled solid SERS substrate with 4-MPy molecules for in situ pHe sensing during apoptosis. We found a more acidic extracellular environment of cancer cells than that of normal cells from the pH imaging. We then in situ investigated the temporal and spatial evolution of pHe of cancer cells after addition of transforming growth factor-β (TGF-β). The pHe showed a fast decrease at the beginning, followed by a slow decrease until the complete loss of cellular functions and the pH values in and out of the cells became similar. This work shows that our SERS substrate combined with in situ cell culture system is well suitable for in situ pHe sensing during cell processes and will be a promising technique for understanding more pHe-related biological and pathological issues.

Research paper thumbnail of Amplified voltammetric detection of miRNA from serum samples of glioma patients via combination of conducting magnetic microbeads and ferrocene-capped gold nanoparticle/streptavidin conjugates

Biosensors & bioelectronics, Jan 5, 2016

MicroRNA (miRNA) plays a key regulatory role in many biological processes, emerging as an importa... more MicroRNA (miRNA) plays a key regulatory role in many biological processes, emerging as an important biomarker for a large variety of cancer diseases. Employing gold nanoparticle (AuNP)-coated magnetic microbeads (AuNP-MMBs) as an immobilization matrix for higher loading density of hairpin-structured DNA probes and then ferrocene (Fc)-capped gold nanoparticle/streptavidin conjugates, amplified electrochemical assay of miRNA has been performed. In the presence of target miRNA, a novel assembly was formed via linking biotinylated hairpin DNA probe-covered AuNP-MMBs with Fc-capped gold nanoparticle/streptavidin conjugates and then collected by magnetic electrodes for voltammetric detection. The enlarged surface area, good conductivity of AuNP-MMBs and the multiple Fc tags on the electrode surface ensure high sensitivity of the method. The oxidation peak current of Fc tags is proportional to the concentrations of miRNA ranging from 5 fM to 100 fM, and a detection limit of 0.14 fM was ach...

Research paper thumbnail of Surface-enhanced Raman spectroscopy: benefits, trade-offs and future developments

Chemical Science, 2020

Surface-enhanced Raman spectroscopy (SERS) is a vibrational spectroscopy technique with sensitivi... more Surface-enhanced Raman spectroscopy (SERS) is a vibrational spectroscopy technique with sensitivity down to the single molecule level that provides fine molecular fingerprints, allowing for direct identification of target analytes.

Research paper thumbnail of Boosting CO2 Hydrogenation to Formate over Edge‐Sulfur Vacancies of Molybdenum Disulfide

Angewandte Chemie International Edition

Synthesis of formate from hydrogenation of carbon dioxide (CO2) is an atom‐economic reaction but ... more Synthesis of formate from hydrogenation of carbon dioxide (CO2) is an atom‐economic reaction but is confronted with challenges in developing high‐performance non‐precious metal catalysts for application of the process. Herein, we report a highly durable edge‐rich molybdenum disulfide (MoS2) catalyst for CO2 hydrogenation to formate at 200 °C, which delivers a high selectivity of over 99 % with a superior turnover frequency of 780.7 h−1 surpassing those of previously reported non‐precious metal catalysts. Multiple experimental characterization techniques combined with theoretical calculations reveal that sulfur vacancies at MoS2 edges are the active sites and the selective production of formate is enabled via a completely new water‐mediated hydrogenation mechanism, in which surface OH* and H* species in dynamic equilibrium with water serve as moderate hydrogenating agents for CO2 with residual O* reduced by hydrogen. This study provides a new route for developing low‐cost high‐perfor...

Research paper thumbnail of In-situ Raman spectroscopic insight into charge delocalization-improved electrical conductivity in metal–cyanide frameworks

Nanoscale

Raman spectroscopy reveals that the enhancement mechanism of electrical conductivity in Prussian ... more Raman spectroscopy reveals that the enhancement mechanism of electrical conductivity in Prussian Blue induced by K ions is charge delocalization.

Research paper thumbnail of Accelerated interfacial proton transfer for promoting electrocatalytic activity

Chemical Science

Adsorbing 4MPy on Pt surface promotes proton transfer at the interfacial layer, maintaining an op... more Adsorbing 4MPy on Pt surface promotes proton transfer at the interfacial layer, maintaining an optimal interfacial pH and promotes electrocatalytic reactions involving proton-coupled electron transfer (PCET) processes.

Research paper thumbnail of A new type of sealed rechargeable lithium–lithium oxide battery based on reversible LiO2/Li2O2 interconversion

Journal of Materials Chemistry A

A new type of sealed battery via the interconversion of LiO2/Li2O2 was developed on the basis of ... more A new type of sealed battery via the interconversion of LiO2/Li2O2 was developed on the basis of the stabilization of LiO2 on the OR-rGO cathode, and a long life of 700 cycles was achieved.

Research paper thumbnail of Operando Electrochemical Xray Diffraction and Raman Spectroscopic Studies Revealing the Alkali-Metal Ion Intercalation Mechanism in Prussian Blue Analogues

Prussian blue analogues are promising cathode material candidates for aqueous rechargeable metal-... more Prussian blue analogues are promising cathode material candidates for aqueous rechargeable metal-ion batteries. Although great efforts have been made on developing materials, there are still rare reports on optimizing cell performance from mechanistic understanding and studies. Here we unveil the alkali-metal-ion intercalation mechanism in Berlin green with a home-built spectroelectrochemical cell for operando X-ray Diffraction (XRD) and Raman spectroscopies, which allows us to obtain the correlated local structure, crystal structure, redox activity, and potential profiles during the charging and discharging processes. We found that the intercalation of Na+ follows a solid solution mechanism leading to a high capacity, and the intercalation of K+ follows a two-phase transition mechanism showing a high voltage. With this understanding, we propose a new strategy using a Na+/K+ hybrid cation electrolyte to realize both high voltage and energy density. This study offers a unique insight for improving the cell performance from the understanding of the reaction mechanism.

Research paper thumbnail of Photoinduced Charge Transfer from a Semiconductor to a Metal Probed at the Single-Nanoparticle Level

Research paper thumbnail of Sensitive and simultaneous surface plasmon resonance detection of free and p53-bound MDM2 proteins from human sarcomas

The Analyst, 2018

Sensitive SPR determination of free and p53-bound MDM2 proteins from sarcoma tissue extracts was ... more Sensitive SPR determination of free and p53-bound MDM2 proteins from sarcoma tissue extracts was carried out in fluidic channels covered with the consensus ds-DNA/p53 conjugate and the consensus ds-DNA, respectively.

Research paper thumbnail of Multiplexed Electrochemical Detection of MiRNAs from Sera of Glioma Patients at Different Stages via the Novel Conjugates of Conducting Magnetic Microbeads and Diblock Oligonucleotide-Modified Gold Nanoparticles

Analytical Chemistry, 2017

MicroRNAs (miRNAs) serve as diagnostic and prognostic biomarkers for a wide variety of cancers. V... more MicroRNAs (miRNAs) serve as diagnostic and prognostic biomarkers for a wide variety of cancers. Via the novel conjugates of gold nanoparticle-coated magnetic microbeads (AuNP-MMBs) and the diblock oligonucleotide (ODN)-modified AuNPs, multiplexed electrochemical assay of miRNAs was performed. The hybridization to target miRNAs leads to the conformational change of the hairpin-structured ODN probes, and the attachment of the diblock ODN-modified AuNPs was achieved. By examining the oxidation peak currents of methylene blue (MB) and ferrocene (Fc) moieties residing on the diblock ODNs, simultaneous quantification of miRNA-182 and miRNA-381 was conducted. The detection signals were significantly enhanced due to the numerous MB and Fc tags on the AuNPs. The proposed assay was highly selective for discriminating miRNAs with similar sequences and detection limits of 0.20 fM and 0.12 fM for miRNA-182 and miRNA-381, respectively, were achieved. The feasibility of the method for sensitive determination of miRNA-182 and miRNA-381 from serum samples of glioma patients at different stages was demonstrated. The sensing protocol thus holds great potential for early diagnosis and treatment of cancer patients.

Research paper thumbnail of In Situ Imaging of Live-Cell Extracellular pH during Cell Apoptosis with Surface-Enhanced Raman Spectroscopy

Analytical Chemistry, 2018

Extracellular pH (pHe) is an important regulating factor that determines many cellular processes,... more Extracellular pH (pHe) is an important regulating factor that determines many cellular processes, including proliferation, differentiation, and apoptosis. In our previous work, we developed 4-MPy (4-mercaptopyridine) modified Au nanoparticles as intracellular pH sensors based on surface-enhanced Raman spectroscopy (SERS). We herein modified Au nanoparticles-assembled solid SERS substrate with 4-MPy molecules for in situ pHe sensing during apoptosis. We found a more acidic extracellular environment of cancer cells than that of normal cells from the pH imaging. We then in situ investigated the temporal and spatial evolution of pHe of cancer cells after addition of transforming growth factor-β (TGF-β). The pHe showed a fast decrease at the beginning, followed by a slow decrease until the complete loss of cellular functions and the pH values in and out of the cells became similar. This work shows that our SERS substrate combined with in situ cell culture system is well suitable for in situ pHe sensing during cell processes and will be a promising technique for understanding more pHe-related biological and pathological issues.

Research paper thumbnail of Amplified voltammetric detection of miRNA from serum samples of glioma patients via combination of conducting magnetic microbeads and ferrocene-capped gold nanoparticle/streptavidin conjugates

Biosensors & bioelectronics, Jan 5, 2016

MicroRNA (miRNA) plays a key regulatory role in many biological processes, emerging as an importa... more MicroRNA (miRNA) plays a key regulatory role in many biological processes, emerging as an important biomarker for a large variety of cancer diseases. Employing gold nanoparticle (AuNP)-coated magnetic microbeads (AuNP-MMBs) as an immobilization matrix for higher loading density of hairpin-structured DNA probes and then ferrocene (Fc)-capped gold nanoparticle/streptavidin conjugates, amplified electrochemical assay of miRNA has been performed. In the presence of target miRNA, a novel assembly was formed via linking biotinylated hairpin DNA probe-covered AuNP-MMBs with Fc-capped gold nanoparticle/streptavidin conjugates and then collected by magnetic electrodes for voltammetric detection. The enlarged surface area, good conductivity of AuNP-MMBs and the multiple Fc tags on the electrode surface ensure high sensitivity of the method. The oxidation peak current of Fc tags is proportional to the concentrations of miRNA ranging from 5 fM to 100 fM, and a detection limit of 0.14 fM was ach...

Research paper thumbnail of Surface-enhanced Raman spectroscopy: benefits, trade-offs and future developments

Chemical Science, 2020

Surface-enhanced Raman spectroscopy (SERS) is a vibrational spectroscopy technique with sensitivi... more Surface-enhanced Raman spectroscopy (SERS) is a vibrational spectroscopy technique with sensitivity down to the single molecule level that provides fine molecular fingerprints, allowing for direct identification of target analytes.