Research Progress----Shanghai Advanced Research Institute,Chinese Academy of Sciences

Researchers Proposed a Facile Tactic to Enhance Electrocatalytic Conversion of Carbon Dioxide

A research team from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences reported a facile tactic that enables exceedingly efficient CO2 electroreduction to CO by virtue of low-coordination chloride ion (Cl-) adsorption on a silver hollow fiber (Ag HF) electrode.

　　The electrochemical conversion of CO2 into carbon-based fuels and valuable feedstocks by renewable electricity is an attractive strategy for carbon neutrality. CO is the key component of syngas, a mixture of CO and H2 that can be directly converted into various value-added chemicals via well-developed industrial processes such as Fischer-Tropsch synthesis, methanol synthesis, etc. Therefore, CO2 electroreduction to CO is considered to be one of the most promising routes to obtain cost-competitive products.
　　However, due to the low solubility and diffusion coefficient of CO2 in aqueous electrolytes, it remains a challenge to possess a large current density, a high faradaic efficiency and excellent stability for practical applications of CO2 utilization.
　　Motivated by such a challenge, a research team led by Profs. CHEN Wei and WEI Wei from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences reported a facile tactic that enables exceedingly efficient CO2 electroreduction to CO by virtue of low-coordination chloride ion (Cl-) adsorption on a silver hollow fiber (Ag HF) electrode.
　　The results were published in Angew. Chem. Int. Ed. on September 3.
　　On the basis of the high efficient electroreduction CO2 to CO over silver hollow fiber (Ag HF) electrode, the research team further introduced chloride ions into the electrode solution, by means of specific adsorption of chloride ions, the electronic structure of the electrode surface was functionally regulated to inhibit the side reaction of hydrogen evolution (HER).
　　The low-coordination chloride ion (Cl-) adsorption on a silver hollow fiber (Ag HF) electrode reduces CO2 to CO at a stable (>150 h) ampere-level current densities (1 A·cm-2) with a high CO faradaic efficiencies (>92%).
　　Electrochemical experiments, operando Raman combined with density functional theory (DFT) calculations demonstrated that the high concentration Cl- in the electrolyte could be low-coordination adsorbed onto the surface of Ag HF, which not only hinders the occurrence of the HER, but also optimizes the kinetics of CO2 reduction to CO, leading to a better eCO2RR performance, even at the ampere-level current density.
　　This work provides a new strategy for further developing electrocatalytic CO2 systems with high current density, high selectivity and high stability in CO2utilization and chlor-alkali industry.
　　Schematic diagram and electrocatalytic performance of efficient CO2 reduction over silver hollow fiber electrode with chloride ion adsorption (Image by SARI)
　　

2022-09-09 more+

The Big Data Science Center at the Shanghai Synchrotron Radiation Facility: The Dawn of the Scientific Superfacilities

The Big Data Science Center (BDSC) at the Shanghai Synchrotron Radiation Facility (SSRF), Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences, Zhangjiang Laboratory, is the first scientific superfacility in China, and one of the first worldwide. With its state-of-the-art developments it aims to dramatically accelerate and automate the multidisciplinary research of all the users at large national scientific facilities, thus effectively increasing the rate of their scientific discoveries and the resulting technological advancements, with a clear societal impact.

　　 Users at the Shanghai Synchrotron Radiation Facility (SSRF) can seamlessly access the scientific and technological architecture of the Big Data Science Center (BDSC) through thin terminals to take full advantage of all the services offered by the BDSC in real time while running their experiments at the SSRF beamlines.
　　The massive amount of raw data produced nowadays at large scientific facilities creates not only enormous new opportunities but also tremendous challenges. Already, only a small fraction of this multidisciplinary and scientifically complex Big Data are fully analysed and, ultimately, used in scientific publications, and it is predicted that in a few years, conventional data-analysis approaches will be overwhelmed, preventing the users from producing meaningful science from their large-scale experiments.
　　This is a problem for all synchrotron and neutron facilities, as well as for X-ray free-electron laser facilities, where tens of petabytes are produced annually. Beamtime is expensive and the lack of automated data-analysis pipelines reduces beamtime efficiency. This “data deluge” effect [1] has implications for all large scientific facilities worldwide in that it affects fast data collection and storage and curation of the data, including data movement and deposition in a database.
　　We are witnessing the dawn of artificial intelligence (AI), machine learning (ML) and robotic automation within the field of large scientific facilities, generating profound changes in how petabytes of interdisciplinary datasets are intelligently processed, managed, analysed and visualised. The consequent evolution of large scientific facilities into superfacilities enables multimodal user science to confront the Big Data challenges, fundamental for the entire scientific community.
　　The Big Data Science Center (BDSC) at the Shanghai Synchrotron Radiation Facility (SSRF), Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences, Zhangjiang Laboratory, is the first scientific superfacility in China, and one of the first worldwide [2]. With its state-of-the-art developments it aims to dramatically accelerate and automate the multidisciplinary research of all the users at large national scientific facilities, thus effectively increasing the rate of their scientific discoveries and the resulting technological advancements, with a clear societal impact. Therefore, the BDSC Big Data Science platform targets the research projects that several national and international universities, academies, research institutes and industries are pursuing at SSRF, where massive support in terms of scientific computation is required to enable the most complete knowledge transfer from scientific research to industrial developments, while elastically interfacing them with the top Chinese National Supercomputer Centers. [video:BDSC - IUCr - LowRes]
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　　Video documentary showing the BDSC activities, international potential and impact on the user’s science at the SSRF, and more in general on the large national scientific facilities worldwide. Here, the BDSC state-of-the-art superfacility capabilities are demonstrated using the Biological Macromolecular Crystallography Beamline (MX Beamline) as a case study, including users performing a real experiment in real time. The entire BDSC workflow is shown, from the preparation of the user experiment at the beamline, through the setting-up of the beamline, to the real-time Big Data analysis and results visualisation, including the user’s data being processed and monitored through the BDSC superclusters and Control Room, as well as the users interacting with the BDSC Platform.
　　The BDSC is one of the latest SSRF upgrades resulting from the SSRF Phase II project. The BDSC aims to support all the SSRF beamlines, as well as their national and international users, through its state-of-the-art scientific computational infrastructure, including high-performance computing (HPC), latest-generation storage systems and advanced software platforms. Users and beamlines at the SSRF are thus benefiting, seamlessly, from the most advanced Big Data processing, movement, analysis, results interpretation and visualisation capabilities offered by the BDSC. The BDSC aims, in fact, to support all the SSRF users to produce high-impact science and technology, matching the highest international quality standards, thus further enabling the users to publish their results in top-notch internationally renowned peer-reviewed journals.
　　Professor Alessandro Sepe, Director of the BDSC, has designed and architected this novel Big Data Science platform at SSRF, which allows all its users to fully exploit the scientific and technological potential of the BDSC for their research. The entire BDSC staff supported Professor Sepe’s efforts in developing, deploying and then constantly upgrading the BDSC infrastructure, which is now fully operational. Here, state-of-the-art Big Data science and technologies, AI, internet of things (IoT), real-time unstaffed and remotely controlled experiments, robotic automation, HPC, cloud/fog supercomputing and massive parallelisation are converging on the SSRF through the BDSC’s fully centralised platform, accelerating the user multidisciplinary science performed at SSRF by an outstanding factor of 60, and effectively creating the first-ever world-class user-friendly Chinese superfacility. This is greatly augmenting the interpretation of all the scientific data generated by all the experiments at SSRF. By developing, deploying and upgrading the Big Data Science platform, the BDSC is fostering full robotic automation at the SSRF beamlines, aiming at real-time unstaffed and remotely controlled experiments, while sharing its successful experience with all the other multidisciplinary large facilities worldwide.
　　The Big Data Science platform developed by the BDSC is, in fact, collecting, tagging and tracking large volumes of metadata from all the experiments at SSRF to fully automate the entire large-facility lifecycle. Hundreds of petabytes of scientific data are thus tagged, to be then ingested by neural networks for ML. This remarkable scientific and technological achievement also allows non-expert users at SSRF to obtain scientifically meaningful results in real time, instead of spending months, after returning to their home institutions, processing unstructured raw data. The BDSC is thus effectively extending the use of large national facilities to the largest number of scientific and industrial disciplines ever, dramatically increasing the scientific and technological productivity of large scientific facilities like SSRF, shifting the focus of their users from data science to pure science, thus enabling a true user-science-centric and multimodal infrastructure.
　　The BDSC is also engaged in further expanding the SSRF scientific computational capabilities, directly interfacing, through the BDSC framework, the SSRF with the supercomputers in China, including the Shanghai Supercomputer Center (SSC), with extremely low-latency networks.
　　The BDSC further aims at seeding the Chinese National Scientific Grid based on the platform model being developed at the BDSC.
　　References:
　　[1] C. Wang, U. Steiner & A. Sepe (2018). Synchrotron Big Data Science. Small, 14, 1802291.
　　[2] C. Wang, F. Yu, Y. Liu, X. Li, J. Chen, J. Thiyagalingam & A. Sepe (2021). Deploying the Big Data Science Center at the Shanghai Synchrotron Radiation Facility: the first superfacility platform in China. Mach. Learn.: Sci. Technol. 2, 035003.
　　
　　Source: International Union of Crystallography (IUCr)
　　

2022-09-07 more+

Novel Approach to Fabricating Gadolinium Oxide Structure Neutron Absorber by 3D Printing

A research team at Shanghai Advanced Research Institute proposed a new approach to fabricating the Gd2O3 structure by vat photopolymerization 3D printing.The research results were published in Ceramics International.

2022-08-29 more+

Novel Approach to 3D Printed Nickel-based Electrocatalysts for Highly-efficient Hydrogen Evolution

A research team at Shanghai Advanced Research Institute reported a novel photo-curing 3D-printing method to manufacture directly the structured nickel-based electrocatalysts with unique gluten-like cubic structure and strong catalyst-substrate interaction.The research results were published in Nano Energy.

Water electrolysis has proved to be an effective method of producing hydrogen employing renewable sources of energy, contributing the national commitment to carbon peak and carbon neutrality.The development of cost-effective electrocatalysts for efficient and durable hydrogen evolution reaction (HER) in alkaline media is of vital importance to meet the increasing demand of hydrogen. The platinum group metals (PGMs) exhibit excellent activity towards the HER, but their high cost hinders their widespread application.Motivated by such a challenge, a research team led by Prof. TANG Zhiyong and Associate Prof. ZHANG Jie at Shanghai Advanced Research Institute reported a novel photo-curing 3D-printing method to manufacture directly the structured nickel-based electrocatalysts with unique gluten-like cubic structure and strong catalyst-substrate interaction.The research results were published in Nano Energy.The photo-curing 3D printing has much lower manufacturing cost than the selective laser melting (SLM) 3D printing, and much higher degree of freedom and printing accuracy than that of direct ink writing (DIW) 3D printing.Based on this technology, researchers optimized printing paste composition and post-treatment process. The resultant electrode surface exhibits gluten-like cubic structure, where Ti exists in amorphous state with strong interaction with Ni, leading to increased active sites and greatly improved electrolytic properties.The tailored Ti-Ni NS electrode exhibits excellent durability and a remarkable low overpotential, surpassing the commercial Pt/C catalyst and most of the state-of-the-art electrocatalysts.Density functional theory (DFT) calculations further reveal that the Ti doping significantly decreases the energy barrier of water dissociation and hydrogen energy barrier, thus enhancing the HER.This work provides a novel strategy to precisely prepare the structured noble-metal-free catalysts with enhanced activity in alkaline water electrolysis(AWE). Moreover, the developed photo-curable 3D printing method provides an alternative option for manufacturing low-cost electrocatalysts with complex 3D architecture.
　　Schematic illustration of photo-curing 3D printing of Ni-based electrode (Image by SARI)
　　

2022-08-12 more+

A Novel Approach for Generating Coherent and Ultrashort Soft X-ray Pulses

A research team from Shanghai Advanced Research Institute reported on the first demonstration of an external seeding mechanism, termed echo-enabled harmonic cascade (EEHC) for generating coherent and ultrashort soft x-ray pulses.

Generation of intense, tunable, and fully coherent pulses in the X-ray regime has been a long-standing challenge for laser technologies. The urgent need for intense X-ray light sources has prompted the development of X-ray free-electron lasers (FELs). However, most of the presently existing X-ray FEL facilities are faced with limited temporal coherence and large shot-to-shot fluctuations.
　　An efficient way to generate ‘laser-like’ FEL is to employ an external laser source as the ‘seed’ to dominate the gain process and control the output properties. Current limitations on seeded FELs are the low harmonic up-conversion efficiency (limits the short wavelength coverage) and long output pulse duration (determined by the length of the external laser).
　　To overcome the above-mentioned limitations of seeded FELs, a research team from Shanghai Advanced Research Institute reported on the first demonstration of an external seeding mechanism, termed echo-enabled harmonic cascade (EEHC) for generating coherent and ultrashort soft x-ray pulses.
　　The results were published in Optica.
　　The EEHC mechanism uses echo-enabled harmonic generation as the first stage, producing intense extreme ultraviolet pulses that seed the second stage x-ray free-electron laser (FEL) with the high-gain harmonic generation setup. The mechanism shows that 100 MW-level peak power, transform-limited soft X-ray pulses with tunable pulse duration from 25 fs to 55 fs can be generated. Comparing with previous demonstrated seeded FEL mechanisms, EEHC holds the superiorities of much higher harmonic up-conversion efficiency and tunable pulse durations.
　　Besides the temporal coherence, researchers have also demonstrated a unique feature of EEHC on generating isolated ultrashort pulses. The supreme up-frequency conversion efficiency and flexible pulse length control of this EEHC mechanism allows to exceed the current limitations of seeded FELs while preserving the coherence of the seed.
　　These features of EEHC are a step towards fully coherent and ultrashort x-ray lasers and could unlock the door for extending nonlinear optical techniques to the sub-nanometer wavelength and few-femtosecond time duration range.
　　Fig. 1 FEL gain curves for the first- (left) and second-stages (Image by SARI)
　　

2022-08-08 more+

Researchers Develop Novel Au Catalyst for Hydroformylation

A research team from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences designed a zeolite-encaged Au single-atom catalyst with Au1-O-SiOX motifs, which shows remarkable catalytic activity and selectivity towards propene hydroformylation.

　　As one of the largest-volume industrial chemical processes today, hydroformylation converts olefins, H2 and CO into aldehydes and related products more than 10 million tons annually.
　　Although Au exhibits good ability towards olefins activation, H2 dissociation and CO bonding, it is conventionally considered inactive for hydroformylation due to its intrinsic inertness.
　　Now, a research team led by Profs. WANG Hui and SUN Yuhan from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences designed a zeolite-encaged Au single-atom catalyst with Au1-O-SiOX motifs, which shows remarkable catalytic activity and selectivity towards propene hydroformylation.
　　The study was published in Chem Catalysis on July 13.
　　Preliminary performance evaluation of impregnated Au on zeolite demonstrates that sub-nanometer Au clusters exhibit higher activity than nanoparticles in hydroformylation. Inspired by this, the confinement effect of zeolite is utilized to regulate the particle size of Au. Nanoparticles/sub-nanoclusters and atomically dispersed Au species within zeolite can be unambiguously observed through high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM).
　　The Au1@S-1 catalyst shows a total 3,794 μmol butyraldehyde and noticeable stability after 5 cycles, which is about one order of magnitude more active than Au nanoparticles and is even comparable to Rh-based catalysts.
　　Detailed characterizations and theoretical calculations indicate that the isolated Au atoms within the zeolite matrix are stabilized via oxygen bridge bonds. The formed Au1-O-SiOX motifs render maximum active site density and high structural stability, which are identified as the real active sites for efficient hydroformylation.
　　This work makes conventionally inactive Au efficient alternative for hydroformylation by reasonably tailoring the size, contact structure and electronic environment of active metals on specific reactions.
　　Structural modeling and performance comparison of Au-based catalysts (Image by SARI)
　　

2022-07-14 more+