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Unveiling the promotion role of ZnO on Zn-Al spinel oxide for CO2 hydrogenation

Journal of Energy Chemistry 2025年第1期100卷 18-25页

作者： Tongyao Wang Xinlong Yao Lixin Liang Hongyu Chen Pan Gao Guangjin Hou State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO2hydrogenation. However, the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates. In this study, we prepared two Zn-Al spinel oxide catalysts via coprecipitation（ZnAl-C）and hydrothermal（ZnAl-H） methods, and conducted a comparative investigation in the CO2hydrogenation reaction. Surprisingly, under similar conditions, ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H. Comprehensive characterizations using X-ray diffraction（XRD）, Raman spectroscopy and electron paramagnetic resonance（EPR） unveiled that ZnAl-C catalyst had abundant ZnO species on its surface, and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies, which are crucial for CO2adsorption and activation. Additionally, state-of-the-art solid-state nuclear magnetic resonance（NMR） techniques,including ex-situ and in-situ NMR analyses, confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species, which was readily hydrogenated to methanol and DME. These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO2-to-methanol hydrogenation reaction, which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst. These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.

关键词： Reaction intermediates

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Formamidinium-incorporated Dion-Jacobson phase 2D perovskites for highly efficient and stable photovoltaics

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Journal of Energy Chemistry 2021年第6期30卷 632-638,I0015页

作者： Sajjad Ahmad Wei Yu Ruixue Lu Yang Liu Tonggang Jiu Shuping Pang Xin Guo Can Li State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian National Laboratory for Clean EnergyDalian 116023LiaoningChina Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina University of Chinese Academy of Sciences Beijing 100049China Department of Chemistry Fudan UniversityShanghai 200438China

Dion-Jacobson phase two-dimensional(DJ 2D)perovskites,recently attracting considerable interests,exhibit excellent environmental stability and structural tunability,but their solar cells still offer unsatisfactory power conversion efficiencies(PCEs).Herein,we develop DJ 2D perovskites employing formamidinium(FA+)as a ternary cation in the perovskite cages((PDA)(FA)x(MA)3-xPb4 I13,χ=0,0.15,0.3 and 0.6,PDA=1,3-propanediammonium)for highly efficient and stable perovskite solar cells(PSCs).We found that the DJ 2D perovskite with a 10%FA+fraction presents improved crystallinity,preferred vertical orientation,and longer charge carrier lifetime compared to that without FA+*** a result,the FAdoped DJ 2D PSCs exhibit a champion PCE of 14.74%with superior device *** unencapsulated devices sustain over 92%of its initial PCE after storage at a constant relative humidity(RH)of 65%for 6000 h,90%by heat at 85℃in air for 800 h,and 94%under 1-sun illumination for 5000 *** findings demonstrate that the incorporation of FA cation into the DJ 2D perovskite is a promising strategy to develop highly efficient and stable DJ 2D PSCs.

关键词： Dion-Jacobson 2D perovskites Perovskite solar cells Formamidinium doping Power conversion efficiency

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Platinum in-situ catalytic oleylamine combustion removal process for carbon supported platinum nanoparticles

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Journal of Energy Chemistry 2020年第2期29卷 120-125页

作者： Qingying Zhao Huanqiao Li Xiaoming Zhang Shansheng Yu Suli Wang Gongquan Sun Division of Fuel Cells and Battery Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina2 University of Chinese Academy of Sciences Beijing 100049China Department of Materials Science Jilin UniversityChangchun 130012JilinChina

Colloidal synthesis method such as oleylamine(OAm)-stabilized process is of great interest for obtaining uniform and highly dispersed platinum nanoparticle catalysts, yet the ligand may unavoidably inhibit their electro-catalytic performance. Thus, fully removing these ligands is critical to activate catalyst surface. Previous research of OAm removal process pointed that thermal annealing was the most effective way in comparison with other methods such as chemical washing, UV–Ozone irradiation and cyclic voltammetry sweeping, but generally resulting in undesired growth of platinum nanoparticle. Few studies concerning a more efficient ligand removal process have been published yet. In this work we proposed a platinum in-situ catalytic OAm combustion strategy to elucidate the removal mechanism of OAm ligands in thermal process and the key experimental parameters were also optimized. In addition, heat flow signal based on differential scanning calorimetry(DSC) measurement as a sensitive indicator, is suggested to reveal the ligand removal efficiency, which is much more reliable than the traditional *** comparison with commercial Pt/C sample, such a surface clean Pt/C electrocatalyst has shown an enhanced specific activity for oxygen reduction reaction. Our removal strategy and the evaluation method are highly instructive to efficient removal of different organic ligands.

关键词： Ligand removal Platinum in-situ catalytic OAm combustion Carbon supported platinum electro-catalyst ORR

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Remarkable difference of phospholipid molecular chirality in regulating PrP aggregation and cell responses

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Chinese Chemical Letters 2023年第2期34卷 236-243页

作者： Cunli Wang Xue Wang Dongdong Wang Shengxu Qian Fusheng Zhang Mingyang Li Minmin Li Wenqi Lu Bo Liu Guangyan Qing School of Biomedical Engineering Dalian University of TechnologyDalian 116024China CAS Key Laboratory of Separation Science for Analytical Chemistry Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of Chemistry and Chemical Engineering Wuhan Textile UniversityWuhan 430200China

Prion diseases are fatal neurodegenerative diseases that can cause severe *** misfolding and accumulation of the prion peptide (PrP)_(106–126) is crucial,and this process is closely relevant to biological ***,how PrP_(106–126)aggregation is affected by the molecular chirality of phospholipid membrane is ***,in this study,a pair of L-and D-aspartic acid (Asp)-modified 1,2-dipalmitoyl-sn–glycero-3-phosphoethanolamine (DPPE) were synthesized to construct chiral *** discover that L-Asp-DPPE liposomes strongly inhibit the oligomerization and amyloidogenesis of PrP_(106–126),whether acting on monomers or oligomers,which rescues cytotoxicity induced by PrP_(106–126).By comparison,D-Asp-DPPE liposomes inhibit peptide oligomerization only at a high concentration and cannot prevent amyloidogenesis when acting on oligomers,which lead to pronounced *** experiment,dynamic change of intracellular Ca^(2+)(_(i)Ca^(2+)) and Ca^(2+)release from endoplasmic reticulum(ER),reactive oxygen species (ROS) production,adsorption dynamics and affinity tests,and fluorescent imaging clearly disclose that molecular chirality of the liposomes dominates conformational transition of PrP_(106–126)from random coil to β-sheet,binding and adsorption of the monomers and oligomers,and subsequent fibrillation process,resulting in distinct inhibition effect in Ca^(2+)overload and release,ROS production and cell *** work is the first to report that interfacial molecular chirality is a potentially crucial influence on the fibrillation process of PrP_(106–126) and its cell responses,whereas the convergence of chiral amino acids and liposomes can be considered potential inhibitors in prion diseases.

关键词： Prion disease Liposome Chirality Interface Cytosolic Ca^(2+)

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A general bimetal-ion adsorption strategy to prepare nickel single atom catalysts anchored on graphene for efficient oxygen evolution reaction

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Journal of Energy Chemistry 2020年第4期29卷 52-57页

作者： Yingqi Xu Weifeng Zhang Yaguang Li Pengfei Lu Zhong-Shuai Wu Hebei Key Lab of Optic-electronic Information and Materials The College of Physics Science and TechnologyHebei UniversityBaoding 071002HebeiChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Single-atom catalysts (SACs) supported on two-dimensional (2D) materials are highly attractive for maximizing their catalytic ***,graphene based SACs are primarily bonded with nitrogen and carbon sites,resulting in poor performance for the oxygen evolution reaction (OER).Herein,we develop a general bimetal-ion adsorption strategy for the synthesis of individually dispersed Ni SACs anchored on the oxygenated sites of ultrathin reduced graphene oxide as efficient OER *** resultant Ni SACs for OER in alkaline electrolyte exhibit a highly stable overpotential of 328 mV at the current density of 10 mA cm^-2,and Tafel slope of 84 mV dec^-1 together with long-term durability and negligible degradation for 50 h,which is greatly outperform its counterparts of nitrogen bonded Ni SACs (564 mV,364 mV dec^-1) and Ni(OH)2 nanoparticles anchored on graphene (450 mV,142 mV dec^-1),and most reported Ni based OER ***,the extended X-ray absorption fine structure at the Ni K-edge and theoretical simulation reveal that the nickel-oxygen coordination significantly boost OER ***,this work will open numerous opportunities for creating novel-type 2D SACs via oxygen-metal bonding as highly robust OER catalysts.

关键词： Single atom catalyst Nickel Graphene Oxygen evolution reaction Electrocatalysts

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Controlling phase transfer of molybdenum carbides by various metals for highly efficient hydrogen production

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Journal of Energy Chemistry 2021年第11期30卷 191-197,I0005页

作者： Xingtao Sun Jiafeng Yu Xin Tong Meng Yang Jixin Zhang Jian Sun Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

The α phase Mo carbide has been widely investigated recently for its high activity in hydrogen production from water gas shift (WGS) reaction. However, high loading of noble metals as well as high economic and environmental cost derived from high-temperature ammonification and carbonization process will lead to high cost of hydrogen production. Thus, the efficient controlling of phase transfer is promising. Herein, metals (Au, Pt, Rh, Cu) with a wide range of loadings were impregnated on flame spray pyrolysis (FSP) made MoO_(3) to produce Mo carbides by one-step carbonization. A breakthrough high metal-normalized hydrogen production rate of 213 mmol H2·gmetal^(-1)·s^(-1) was achieved on 0.025 wt% Rh/MoCx, which was much higher than Pt and Au based Mo carbides ever reported. The addition of trace Rh induced direct MoO_(3) transformation to high purity α-MoC_(1-x) in one-step carbonization instead of two-steps ammonification and carbonization process. In comparison to Rh, the addition of Pt, Au and Cu tend to transfer MoO_(3) into β-Mo2C at the same conditions. Besides, the one with 2 wt% Rh exhibited high stability in WGS reaction even at high temperature (300 ℃) due to its inhibition on carbides oxidation induced by H2O. We demonstrate that it is feasible to control phase transfer of Mo carbides even by trace amount of metals to simplify the production process of catalysts. The catalytic performance improved by Rh in aspects of both activity and stability provides a guide for producing more stable Mo carbides catalysts.

关键词： Mo carbides α-MoC1-x Stability WGS Hydrogen production

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Difluoroalkylative carbonylation of alkenes to access carbonyl difluoro-containing heterocycles:convenient synthesis of gemigliptin

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Science China Chemistry 2023年第1期66卷 139-146页

作者： Zhi-Peng Bao Youcan Zhang Le-Cheng Wang Xiao-Feng Wu Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Leibniz-Institut für Katalyse e.V.Albert-Einstein-Straße 29a Rostock 18059Germany

Fluorinated heterocycles play a vital role in pharmaceutical and agrochemical ***,rapid and efficient construction of fluorinated heterocycles remains highly ***,a difluoroalkylative carbonylative cyclization of unactivated alkenes and ethylene gas enabled by palladium catalysis has been developed for the first time toward the synthesis ofα-carbonyl difluoro-modified *** procedure can also be applied to the synthesis of Ge Migliptin which is a medicine approved for the treatment of type 2 diabetes mellitus.

关键词： difluoroalkylative carbonylative unactivated alkenes ethylene gas heterocycles

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Using expansion units to improve CO_(2) absorption for natural gas purification——A study on the hydrodynamics and mass transfer

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Chinese Journal of Chemical Engineering 2021年第1期34卷 35-46页

作者： Kai Zhu Chaoqun Yao Yanyan Liu Guangwen Chen Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

The usage of capillary tubes for CO_(2) absorption suffers from small re sidence time,which leads to reduced performance for large *** work presents a method of connecting expansion units to capillary tubes to serve as a residence time *** effect of the expansion unit on gas-liquid hydrodynamics,pressure drop and mass transfer coefficient(k_(L)a) are investigated under various operating pressures up to 4.0 MPa,for both physical and chemical absorption.A novel periodic jetting flow is found in the expansion unit,which can intensify the CO_(2) *** results show that the strategy can significantly decrease the pressure drop while maintaining the absorption performance to a large *** overall k_(L)a for physical and chemical absorption are correlated to pressure drop,***,CO_(2) loading in rich absorbents increases dramatically compared to literature studies with only micromixers or capillary tubes,which is bene ficial to regenerate *** study verifies the concept that pre-treatment with water can largely reduce the usage of amine s,and can also provide a guide for process design in natural gas purification such as biogas recovery.

关键词： Microchannel Microreactor Separation Purification High pressure

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Pt@h-BN core-shell fuel electrocatalysis confined cell electrocatalysts wit under outer shells

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Nano Research 2018年第6期11卷 3490-3498页

作者： Mengmeng Sun Jinchao Dong Yang Lv Siqin Zhao Caixia Meng Yujiang Song Guoxiong Wang Jianfeng Li Qiang Fu Zhongqun Tian Xinhe Bao State Key Laboratory of Catalysis iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China University of Chinese Academy of Sciences Beijing 100049 China MOE Key Laboratory of Spectrochemical Analysis and Instrumentation State Key Laboratory of Physical Chemistry of Solid Surfaces iChEM College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 China

Two-dimensional （2D） materials such as graphene and hexagonal boron nitride （h-BN） can be used as robust and flexible encapsulation overlayers, which effectively protect metal cores but allow reactions to occur between inner cores and outer shells. Here, we demonstrate this concept by showing that Pt@h-BN core-shell nanocatalysts present enhanced performances in H2/O2 fuel cells. Electrochemical （EC） tests combined with operando EC-Raman characterizations were performed to monitor the reaction process and its intermediates, which confirm that Pt-catalyzed electrocatalytic processes happen under few-layer h-BN covers. The confinement effect of the h-BN shells prevents Pt nanoparticles from aggregating and helps to alleviate the CO poisoning problem. Accordingly, embedding nanocatalysts within ultrathin 2D material shells can be regarded as an effective route to design high-performance electrocatalysts.

关键词： electrocatalysis two-dimensional materials core-shell confinement catalysis operando Raman

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A perspective on graphene for supercapacitors: Current status and future challenges

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Journal of Energy Chemistry 2021年第2期30卷 354-357,I0012页

作者： Feng Su Zhong-Shuai Wu Dalian National Laboratory for Clean Energy.Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Supercapacitors,also known as ultracapacitors or electrochemical capacitors,possess intriguing merits of high power density(10-100 times higher than that of batteries),long life expectancy(millions of cycles),wide ope... 详细信息

关键词： Graphene Supercapacitors Energy storage Electric double layer capacitors Pseudocapacitors Hybrid supercapacitors

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