Ruru Chen

Chinese Academy of Sciences

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Rong Cao

Fujian Institute of Research on the Structure of Matter

Minna Cao

Fujian Institute of Research on the Structure of Matter

Yanqiang Huang

Dalian Institute of Chemical Physics

Hongfang Li

Fujian Institute of Research on the Structure of Matter

Hongfang Li

Shanghai Jiao Tong University

Jin-Yun Wang

Chinese Academy of Sciences

Huimin Wang

Ministry of Agriculture and Rural Affairs

Dongxia Yan

Institute of Process Engineering

Jian Zhao

Liaoning Normal University

Brian Brun Hansen

Technical University of Denmark

Cooperative Institutions

Chinese Academy of Sciences

185

University of Chinese Academy of Sciences

137

Beijing Institute of Genomics

Shanghai Center For Bioinformation Technology

Sun Yat-sen University

Huazhong University of Science and Technology

Shanghai Jiao Tong University

Chinese Academy of Medical Sciences & Peking Union Medical College

Peking University

Sichuan University

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Secondary Coordination Sphere Engineering of Single‐Sn‐Atom catalyst via P Doping for Efficient CO₂ Electroreduction

Advanced Energy Materials (2024)

Caizhen Yue Xiaobo Yang Xiong Zhang Shifu Wang Wei Xu

Abstract The regulation of the local microenvironment in the single‐atom catalysts affords a scheme for accelerating the overall reaction kinetics of electrochemical CO 2 reduction reaction (CO 2 RR), which is of vital importance but remains challenging. Herein, a carbon nanotube‐supported single‐Sn‐atom catalyst (P‐SnN 4 ‐CNT) is developed by a modified pyrolysis procedure with P‐doping into the second coordination shell of SnN 4 moiety to modulate the electron structure of metal Sn center. The resulting P‐SnN 4 ‐CNT delivered a high CO partial current density of −380 mA cm −2 with Faradaic efficiency (FE) of CO above 90% across a wide range of −0.5 to −0.8 V versus reversible hydrogen electrode (vs RHE), along with optimal FE (CO) of ≈98.5% at −0.6 V versus RHE in a flow cell. Moreover, P‐SnN 4 ‐CNT achieved an extremely high turnover frequency of 126 471 h −1 with an applied potential of −0.8 V versus RHE, which ranks the best among the reported M─N─C catalysts for electrocatalytic CO 2 reduction. The combination of in situ characterization techniques and density functional theory calculation revealed that the doping of P atoms benefited the activation and hydrogenation steps of CO 2 and promoted the Sn 4+ reduction to Sn 2+ during the reaction process, where Sn 2+ is identified as the active site for the CO generation. The work provides a clear mechanistic insight for both electron structure optimization and identification of active sites by local microenvironment regulation of single‐Sn‐atom, which shall pave a way for the exploitation of other M─N─C catalysts with high CO 2 RR performance.

Coordination sphere

10.1002/aenm.202401448

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Operando Mössbauer Spectroscopic Tracking the Metastable State of Atomically Dispersed Tin in Copper Oxide for Selective CO₂ Electroreduction

Journal of the American Chemical Society (2023)

Ruru Chen Jian Zhao Yifan Li Yi Cui Ying‐Rui Lu

Metastable state is the most active catalyst state that dictates the overall catalytic performance and rules of catalytic behaviors; however, identification and stabilization of the metastable state of catalyst are still highly challenging due to the continuous evolution of catalytic sites during the reaction process. In this work, operando119Sn Mössbauer measurements and theoretical simulations were performed to track and identify the metastable state of single-atom Sn in copper oxide (Sn1-CuO) for highly selective CO2 electroreduction to CO. A maximum CO Faradaic efficiency of around 98% at -0.8 V (vs. RHE) over Sn1-CuO was achieved at an optimized Sn loading of 5.25 wt. %. Operando Mössbauer spectroscopy clearly identified the dynamic evolution of atomically dispersed Sn4+ sites in the CuO matrix that enabled the in situ transformation of Sn4+-O4-Cu2+ to a metastable state Sn4+-O3-Cu+ under CO2RR conditions. In combination with quasi in situ X-ray photoelectron spectroscopy, operando Raman and attenuated total reflectance surface enhanced infrared absorption spectroscopies, the promoted desorption of *CO over the Sn4+-O3 stabilized adjacent Cu+ site was evidenced. In addition, density functional theory calculations further verified that the in situ construction of Sn4+-O3-Cu+ as the true catalytic site altered the reaction path via modifying the adsorption configuration of the *COOH intermediate, which effectively reduced the reaction free energy required for the hydrogenation of CO2 and the desorption of the *CO, thereby greatly facilitating the CO2-to-CO conversion. This work provides a fundamental insight into the role of single Sn atoms on in situ tuning the electronic structure of Cu-based catalysts, which may pave the way for the development of efficient catalysts for high-selectivity CO2 electroreduction.

Metastability

Tin oxide

Copper oxide

10.1021/jacs.3c06738

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Citations (37)

CCDC 2014664: Experimental Crystal Structure Determination

The Cambridge Structural Database (2022)

Xianmeng Song Minna Cao Ruru Chen Huimin Wang Hongfang Li

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

10.5517/ccdc.csd.cc25mf5f

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CCDC 2014662: Experimental Crystal Structure Determination

The Cambridge Structural Database (2022)

Xianmeng Song Minna Cao Ruru Chen Huimin Wang Hongfang Li

10.5517/ccdc.csd.cc25mf3c

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Recent greening of grasslands in northern China driven by increasing precipitation

Journal of Plant Ecology (2021)

Kai Di Zhongmin Hu Mei Wang Ruochen Cao Minqi Liang

Abstract Aims Recent warmer and wetter climate in northern China remains a hot topic in recent years, yet its effect on vegetation growth has not been fully understood. This study investigated the temporal change of vegetation cover and its correlations with climatic variables from 1982 to 2018 for grasslands in northern China. Our aim is to clarify whether the warmer and wetter climate in recent years drives the greening of the vegetation in this region. Methods We investigated the temporal dynamic of vegetation normalized difference vegetation index (NDVI) and its driving forces based on long time-series data. Piecewise regression was used to examine whether there was a turning point of the trend of NDVI and climatic variables. Pearson correlation analyses were conducted to quantify the relationship between NDVI and climatic factors. Stepwise multivariable regression was used to quantify the contributions of climate variables to the temporal variations in NDVI. Important Findings We found a turning point of NDVI trend in 2008, with GIMMS NDVI indicating a slight increase of 0.00022 yr−1 during 1982–2008 to an increase of 0.002 yr−1 for GIMMS NDVI during 2008–2015 and 0.0018 yr−1 for MODIS NDVI during 2008–2018. Precipitation was the predominant driver, and air temperature and vapor pressure deficit exerted a minor impact on the temporal dynamics of NDVI. Overall, our results suggest a turning point of NDVI trend, and that recent warmer and wetter climate has caused vegetation greening, which provides insights for better predicting the vegetation cover in this region under changing climate.

10.1093/jpe/rtab036

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Citations (9)

CCDC 1921936: Experimental Crystal Structure Determination

The Cambridge Structural Database (2019)

Ruru Chen Minna Cao Jin-Yun Wang Hongfang Li Rong Cao

10.5517/ccdc.csd.cc22hxyg

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Degradation Behavior and Immunological Detection of Silk Fibroin Exposure to Enzymes

Analytical Sciences (2019)

Ruru Chen Lian Zhou Hui Yang Hailing Zheng Yang Zhou

The degradation behavior of silk fibroin (SF) is a significant and intriguing subject in the area of archaeological ancient silk research. In the present study, the immunological detection techniques combined with traditional characterization methods, jointly studied the degradation process of SF from Bombyx mori (B. mori) and Antheraea pernyi (A. pernyi) through exposure to alkaline proteinase, α-chymotrypsin, pepsin, and trypsin. Spectroscopic analysis revealed that different enzymes showed similar hydrolysis effects on the secondary structure, but the changes of B. mori SF and A. pernyi SF were mainly reflected in the decrease of β-sheet and the reduction of α-helical structure, respectively. In further research of immunology, two diagnostic antibodies were prepared corresponding to SF of B. mori and A. pernyi, respectively. The enzyme-linked immunosorbent assay (ELISA) and western blot indicated the enzyme-treated SF proteins still exhibited higher immunoreactivity because the epitopes on the surface of SF molecules are retained. Although α-chymotrypsin possesses the most cleavage sites among these enzymes, the α-chymotrypsin-treated SF did not exhibit significant changes in secondary structures and high antibody binding capacity. The results deepen our understanding of the SF degradation process during enzymatic hydrolysis, and show far-reaching guiding significance in trace detection of SF.

Antheraea pernyi

Fibroin

Bombyx

Cleavage (geology)

10.2116/analsci.19p222

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Citations (12)

Base‐free synthesis of bio‐derived 2,5‐furandicarboxylic acid using SBA‐15 supported heteropoly acids in ionic liquids

ChemistrySelect (2022)

Ruru Chen Qiu Zhao Dongxia Yan Jiayu Xin Xingmei Lü

Abstract 2,5‐Furandicarboxylic acid (FDCA) is a green and renewable substitute to terephthalic acid (TPA), the fundamental monomer of polyethylene terephthalate (PET) plastic. This work investigated novel supported Keggin phosphormolybdic acids (HPMs) for the synthesis of FDCA from 5‐hydroxymethylfurfural (HMF) in imidazole ionic liquids. Among four supporters, Al 2 O 3 , SiO 2 , ZSM‐5 and SBA‐15, SBA‐15 exhibited highest stability and specific surface area 507 m 2 /g. FDCA yield achieved 76 % by using HPM/SBA‐15, and maintained 60 % after 5 runs. Particularly, [Bmim]Cl ionic liquid was stable both in thermal and chemical properties by confirmation of FTIR and NMR. HPM/SBA‐15 was also employed in different monosaccharides to FDCA, and led to acceptable yields. A moderate FDCA yield of 34 % from glucose was obtained, revealing a great potential of one‐pot synthesis of FDCA from renewable and accessible carbohydrates.

Thermal Stability

Monosaccharide

10.1002/slct.202200529

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Citations (1)

Secondary Coordination Sphere Engineering of Single‐Sn‐Atom catalyst via P Doping for Efficient CO₂ Electroreduction (Adv. Energy Mater. 38/2024)

Advanced Energy Materials (2024)

Caizhen Yue Xiaobo Yang Xiong Zhang Shifu Wang Wei Xu

CO2 Electroreduction In article number 2401448, Jie Yin, Xuning Li, and co-workers achieved a remarkably enhanced CO2RR performance by engineering the secondary coordination sphere of a single-Sn-atom catalyst via P doping. The doping of P atoms promotes the reduction of Sn4+ to Sn2+, with the in-situ generated Sn2+ identified as the true active site for the CO generation.

Coordination sphere

10.1002/aenm.202470166

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Combustion of micron-sized iron particles in a drop tube reactor

Fuel (2024)

Ruru Chen Leon C. Thijs Brian Brun Hansen Weigang Lin Hao Wu

10.1016/j.fuel.2024.133814

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