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    Researchers Construct Post-synthetic Modification of Covalent Organic Frameworks for CO2 Electroreduction

    A research team at the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences constructed a multilevel post-synthetic modification strategy to construct catalytic COFs towards CO2RR with high activity and selectivity. The research results were published in Nature Communications.

    Covalent organic frameworks (COFs), which possess ordered pores and high-precision functionalization, are regarded as an ideal class of templates to construct catalysts for electrocatalytic carbon dioxide reduction reaction (CO2RR). 
    　　The C-N bonds can improve the adsorption of CO2 and ionic skeletons can promote the charge transfer, further enhancing the conductivity. However, directly bottom-up synthesis can hardly realize the co-existence of C-N bonds and ionic frameworks due to the electrostatic repulsion and weak strength of the linkage. 
    　　Motivated by this challenge, a research team led by Prof. ZENG Gaofeng and Associate Prof. XU Qing at the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences constructed a multilevel post-synthetic modification strategy to construct catalytic COFs towards CO2RR with high activity and selectivity. The research results were published in Nature Communications.  
    　　The catalytic COFs synthesised by the post modification show a maximum turnover frequencie value of 9922.68 h–1 at –1.0 V and the highest faradaic efficiencies of 97.32% at –0.8 V, which are higher than that of the base COF and the single-modified COFs. The electrocatalysis tests and characterizations reveal that C-N bonds can improve the catalytic selectivity and ionic skeleton contributes to higher activity. 
    　　Furthermore, the theoretical calculations illustrate that the easier formation of immediate *CO from COOH* is the rate determined step, and methyl groups strengthen the electron density. 
    　　This work provides a deeper understanding of COFs in CO2 reduction reaction. In the meantime, it sheds light on constructing multilevel post-synthetic modification COFs towards tailored activity and high stability.
    　　 
    　　Catalytic covalent organic frameworks with bifunctional roles in oxygen reduction reaction (from O2 to H2O) and oxygen evolution reaction (from H2O to O2) have been first demonstrated by integrating redox-active sites into the Co-porphyrin frameworks. (Image by SARI)
    　　

    2023-06-29 more+

    Scientists Develop a Novel Approach to Support Future Power System

    Large-scale clusters of electric vehicles (EVs) are an important reserve measure supporting the construction of new power system. Key technologies towards the reliable and economic operation require collaborative innovation across disciplines and fields.Driven by the increasing needs, a joint research team led by Shanghai Advanced Research Institute of the Chinese Academy of Sciences proposed a novel approach to support future power system towards global net-zero emission target. The results were published in the latest issue of Renewable and Sustainable Energy Reviews.


    　　The fundamental solution to achieve the "double carbon" goal is to transform the traditional energy consumption toward a low-carbon environment. Therefore, building a new type of power system with new energy sources can guarantee the low-carbon transformation of energy.
    　　Large-scale clusters of electric vehicles (EVs) are an important reserve measure supporting the construction of new power system. Key technologies towards the reliable and economic operation require collaborative innovation across disciplines and fields.
    　　Driven by the increasing needs, a joint research team led by Shanghai Advanced Research Institute of the Chinese Academy of Sciences and Nanjing University of Posts and Telecommunications proposed a novel multidisciplinary approach to support future power system towards global net-zero emission target.
    　　The results were published in the latest issue of Renewable and Sustainable Energy Reviews.
    　　This research group reconciled large-scale electric vehicle clusters into the power grid as a case study, and proposed the framework of interactions with physical flow, behavioral flow and information flow.
    　　They first analyzed the physical characteristics of electric vehicle clusters providing power system reserve from the perspectives of performance characteristics, resource aggregation, scheduling strategies, and market mechanisms.
    　　Then, the importance of social factors was emphasized and a hybrid simulation technology that integrates human participants and computer multi-agents was proposed, to solve the problem of heterogeneity in users’ decision-marking behavior.
    　　In addition, the research group discussed the potential solutions regarding global communication coverage, frequency band interference and avoidance, communication security, and customized priority protection. Based on the perspective of the integration of public/private communication networks with Chinese characteristics, the researchers contrapuntally proposed grant-free transmission strategy, joint differentiated spectrum sensing & frequency hopping scheme, and implicit dimension labeling technique for the challenges above.
    　　The research work provides technical support and feasible directions for multiple types of distributed reserve resources such as large scientific installations, office buildings, and industrial and agricultural production loads, which can enhance the flexible regulation capability of future power systems. It also introduces a feasibility guarantee that enables more distributed reserve resources for future power systems in various countries and regions. 
    　　An illustration of full-domain application of the new electric power system (Image by SARI)
    　　

    2023-06-21 more+

    Novel Approach towards the Fabrication of Artificial GNRs with Pentagon Carbon Embedded

    a research team led by Prof. SONG Fei at Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences reported a novel approach to precisely fabricate well-defined GNRs with the tailored carbon pentagon embedded inside, supported on the Ag(111) model catalyst. The results were published in Journal of Physical Chemistry Letters entitled "On-Surface Synthesis of Pentagon-Incorporated Graphene-Like Nanoribbons with Multiple Precursors”.

    Appealing properties have been awarded to graphene nanoribbons (GNRs) because of their unique electronic structures with high tunability of physical structures. However, the fabrication feasibility of artificially tuned GNRs intrinsically associated with their external properties brings considerable challenges in the synthesis and of GNRs and utilization in devices. 
    　　Motivated by such a challenge, a research team led by Prof. SONG Fei at Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences reported a novel approach to precisely fabricate well-defined GNRs with the tailored pentagon carbon embedded inside, supported on the Ag(111) model catalyst. 
    　　The results were published in Journal of Physical Chemistry Letters entitled "On-Surface Synthesis of Pentagon-Incorporated Graphene-Like Nanoribbons with Multiple Precursors”. 
    　　Compared to the conventional solution-synthesis chemistry, on-surface Ullmann coupling strategy introduces feasibility and controllability on demand towards the atomically precise nanostructures of well-modified GNRS, by programmed cleavage of carbon-halogen bonding in precursors and the reconnection of carbon-carbon bonding on surface. 
    　　Moreover, by utilizing multiple precursors as designed, carbon pentagon structures can be feasibly introduced into GNRs via Ullmann coupling and cyclodehydrogenation on Ag(111), resulting the artificial modification of both nanostructures and electronic structures with the high stability, as witnessed by scanning tunneling spectroscopy (STS) and density function theory (DFT).
    　　This study provides a novel strategy to promote on-surface GNRs-based nanostructures towards field effect transistors (FET), high-density storage devices, etc. 
    　　On-surface synthesis of pentagon-incorporated Graphene Nanoribbons (Image by SARI)
    　　

    2023-06-16 more+

    Researchers Develop Highly Efficient Ampere-Level CO2 Reduction to Multicarbon Products via Stepwise Hollow-Fiber Penetration Electrodes

    Recent studies have shown that serial hollow-fiber penetration electrodes (HPEs) can improve the CO2ERR performance significantly. To promote the selectivity and current density for C2+ products simultaneously, a research team from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences developed a stepwise CO2ERR strategy using Ag and Cu HPEs to reach high-rate C2+ production.The results were published in Appl. Catal. B-Environ. on 28th May, 2023.


    　　Though efficient C2+ production from CO2 electrocatalytic reduction reaction (CO2ERR) has become a promising approach to mitigate CO2 emissions and store intermittent renewable energy, it suffers from low selectivity and undesired side reactions.
    　　Recent studies have shown that serial hollow-fiber penetration electrodes (HPEs) can improve the CO2ERR performance significantly by forcing CO2 to disperse and penetrate through the abundant pores on HPE wall, which greatly boosted CO2ERR kinetics.
    　　To promote the selectivity and current density for C2+ products simultaneously, a research team led by Profs. CHEN Wei and WEI Wei from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences developed a stepwise CO2ERR strategy using Ag and Cu HPEs to reach high-rate C2+ production.
    　　The results were published in Appl. Catal. B-Environ. on 28th May, 2023.
    　　Specifically, for stepwise CO2 electroreduction, CO2 was firstly reduced into CO over a chloride ion regulated Ag hollow-fiber penetration electrodes with a 3.2 A？cm-2 partial current density and a 90.3% faradaic efficiency of CO. Then, a chloride ion regulated Cu hollow-fiber penetration further converted CO into C2+ products with a 1.8 A cm-2 partial current density and a 90.5% faradaic efficiency of C2+ products. Both steps were steadily conducted under total current density of 2 A？cm-2 for 200 hours.
    　　Experimental results and density functional theory calculations show that synergetic combination of the unique penetration effect and the regulated electronic structures resulted in the superior performance toward C2+ production
    　　This work shed light on designing electrocatalytic systems with exceedingly efficient CO2 electroreduction of high current density and selectivity as well as good durability, which might contribute to the scalable CO2 electroreduction applications towards high-value C2+ chemicals.
    　　Schematic diagram for highly efficient ampere-level CO2 reduction to multicarbon products via stepwise hollow-fiber penetration electrodes (Image by SARI)
    　　

    2023-06-05 more+

    Researchers Developed Linkage Engineering of Covalent Organic Frameworks for the Oxygen Reduction Reaction

    A joint team lead by Prof. ZENG Gaofeng and Associate Prof. XU Qing from Shanghai Advanced Research Institute, CAS and Prof. JIANG Zheng from University of Science and Technology of China employed catalytic linkage engineering to modulate the catalytic behaviors and found the catalytic performance is determined solely by the electron states of carbon atoms in the linkages. The research results were published in Angew Chem Int Ed.


    　　Covalent organic frameworks (COFs) are the ideal templates to create metal-free catalysts because of their well-defined porous structures, predictable sites distribution and tailored environments. Attention has been put on employing different knots or linkers to advance the catalytic performance, however, the important roles of linkages toward catalyzing the oxygen reduction reaction (ORR) have not been investigated, and which linkage is more suitable for ORR is still under investigation.
    　　Recently, a joint team lead by Prof. ZENG Gaofeng and Associate Prof. XU Qing from Shanghai Advanced Research Institute, CAS and Prof. JIANG Zheng from University of Science and Technology of China employed catalytic linkage engineering to modulate the catalytic behaviors and found the catalytic performance is determined solely by the electron states of carbon atoms in the linkages.
    　　The research results were published in Angew Chem Int Ed.
    　　Researchers developed catalytic COFs using different bonds such as imine, amide, azine, and oxazole bonds to link benzene units to catalyze ORR. Among these COFs, the oxazole-linkage in COFs enables to catalyze the ORR with the highest activity, which achieved a half-wave potential of 0.75V and a limited current density of 5.5mA cm -2.
    　　Theoretical calculations showed that the carbon atoms in oxazole linkages promoted the formation of the OOH* and OH* intermediates, thus advancing the catalytic activity. This work provides guidance in choosing suitable linkages for ORR. 
    　　Chemical structures of COFs (azine-, imine-, amide-, and oxazole-COF) with different linkages (Image by SARI)
    　　

    2023-06-02 more+

    Researchers Constructed Noninterpenetrated Three-dimensional Covalent Organic Framework for Au Ions Capture

    A research team led by Prof. ZENG Gaofeng and Associate Prof. XU Qing at the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences constructed a novel non-interpenetration 3D COF towards Au ions capture by imine bonds in the frameworks. The research results were published in Adv. Funct. Mater. on Apr. 23rd.

    Covalent organic frameworks (COFs) can be ideal platform for detecting or extracting metal ions because of the different functional building units and large surface area. However, most of 3D COFs have interpenetration because of the existence of non-covalent interactions between the adjacent nets, which resulting in decreased surface areas and porosizes, and thus limited their applications in catalysis and molecular/gas adsorption.Recently, a research team led by Prof. ZENG Gaofeng and Associate Prof. XU Qing at the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences constructed a novel non-interpenetration 3D COF towards Au ions capture by imine bonds in the frameworks. The high surface area and abundant cavities due to the non-interpenetration provided the high Au3+ capacity (570.18 mg g-1), selectivity (99.5%) and efficiency (68.3% adsorption of maximum capacity in 5 mins).The research results were published in Adv. Funct. Mater.on Apr. 23rd. The synthesized BMTA-TFPM-COF displayed good crystallinity with dia topology and a high BET surface area of 1924 m2 g-1. Importantly, the open cavities and exposed C=N bonds from non-fold interpenetration contributed to high capacity, selectivity and stability of Au3+ uptake.The experiments showed the mechanism of Au capture. The protonated C=N bonds due to the influence of the HAuCl4 and the protonated nitrogenous groups could adsorb AuCl4 - and reduce Au(III) to Au(I) and Au(0) in acidic solution. Thus, the BMTA-TFPM-COF with abundant exposed C=N bonds could promote the conversion from Au(III) to Au(I) and Au(0) through the protonated C=N bonds, which further verified that the C=N bonds could participate in the reduction of Au(III).
    　　 Mechanism of 3D COFs (Image by SARI)This study gives new insight into the development of 3D COFs for Au3+ capture. 

    2023-04-28 more+
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