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Efficient epoxidation of propylene over non-noble nickel-based catalyst promoted by alkali metals

science China Chemistry 2024年第11期67卷 3697-3705页

作者： Wenqian Li Wanting Li Xinxin Cao Longfei Chen Yibo Qin Yanfeng Zhu Yanfei Zhang Gai Miao Lingzhao Kong Jiong Li Xinqing Chen State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization CAS Key Laboratory of Low-carbon Conversion Science and EngineeringShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China School of Environmental Science and Engineering Suzhou University of Science and TechnologySuzhou 215009China Shanghai Synchrotron Radiation Facility Zhangjiang National LabShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China

The application of non-noble metal catalysts in the catalytic direct gas-phase epoxidation of propylene with H2and O2to produce propylene oxide is valuable and challenging. The introduction of alkali metal promoters is one of the effective methods to improve the catalytic activity of catalysts. Herein, a series of alkali metal(Li, Na, K, Rb, and Cs)-promoted Ni/TS-1 catalysts were prepared to deeply understand the effect of alkali metals on the structure-activity relationship for gas-phase epoxidation of propylene. Among them, the Na-Ni/TS-1 catalyst exhibits the highest catalytic activity(propylene conversion of 7.35% and PO formation rate of 157.9 g h^(-1)kg_(cat)^(-1)) and the best stability(long-term stability exceeding 140 h at 200 ℃). X-ray absorption and photoelectron spectroscopy revealed that the electronic structure of Ni can be tuned by the addition of alkali metal ***3-TPD-MS, CO_(2)-TPD-MS, and C_(3)H_(6)-TPD-MS results indicate that the acidity of the catalyst can also be adjusted by the introduction of alkali metal, whereas the Na-Ni/TS-1 catalyst exhibits the strongest C_(3)H_(6) adsorption capacity. Thus, the suitable acid-base properties, unique electronic properties of Ni species, and the strongest propylene adsorption capacity resulted in improved propylene gas-phase epoxidation activity of Na-Ni/TS-1 catalyst. This study not only provides a new strategy for the practical application of nickel-based catalysts in the gas-phase epoxidation of propylene but also provides insights into the promoting effect of alkali metals.

关键词： propylene epoxidation Ni/TS-1 catalyst alkali metal precipitating agents

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A justice and innovative way ahead of consumption-based emission accounting approach

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science China Earth sciences 2024年第9期67卷 2999-3010页

作者： Qun SHEN Hongbo DUAN Yun TANG Linbing TANG Li SHANG Xinyu DOU Wei WEI Weiqiang CHEN Zhu LIU State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization CAS Key Laboratory of Low-Carbon Conversion Science&EngineeringShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China School of Economics&Management University of Chinese Academy of SciencesBeijing 100190China Key Lab of Urban Environment and Health Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Department of Earth System Science Tsinghua UnivesityBeijing 100084China

carbon emission accounting is an important basis for global climate *** on the consumption-based accounting(CBA)method,the characteristics of carbon flow between national,regional,and product processes could be more clearly ***,CBA is more conducive to clarifying the attribution of responsibilities between producers and consumers,with the principles of fairness and *** accounting for carbon emissions in typical countries from 1990 to 2019,we found that the CBA emissions are higher than the production-based accounting(PBA)emissions in major developed countries,while the results are reversed for developing *** the past 30 years,the CBA emissions in targeted developed countries generally have shown a downward trend,while in developing countries,they have shown an upward *** emissions in China have shown a continuous growth trend from 1990 to 2019,but the pace has slowed down significantly over the last ***,the embodied carbon intensity of China’s exports continues to decline,indicating that China is providing more green and low-carbon products to the *** the PV industry as an example,this study further reveals the contribution of specific product industries to the country’s carbon transfer through product carbon footprint *** order to provide a scientific basis for global mitigation and climate governance,it is urgent to innovate a scientific,practical,and standardized CBA technology system.

关键词： Consumption-based accounting Production-based accounting carbon transfer carbon footprint

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Metal organic polymers with dual catalytic sites for oxygen reduction and oxygen evolution reactions

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carbon Energy 2023年第5期5卷 127-137页

作者： Sijia Liu Minghao Liu Xuewen Li Shuai Yang Qiyang Miao Qing Xu Gaofeng Zeng CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute(SARI)Chinese Academy of Sciences(CAS)ShanghaiChina School of Physical Science and Technology ShanghaiTech UniversityShanghaiChina School of Chemical Engineering University of Chinese Academy of SciencesBeijingChina

Metal-organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons,controllable porosities,and well-defined catalytic ***,the poor chemical stability and low electron conductivity limited their activity,and single-functional sites in these frameworks hindered them to show multifunctional roles in catalytic ***,we have constructed novel metal organic polymers(Co-HAT-CN and Ni-HAT-CN)with dual catalytic centers(metal-N_(4) and metal-N_(2))to catalyze oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).By using different metal centers,the catalytic activity and selectivity were *** them,Co-HAT-CN catalyzed the ORR in a 4e^(-)pathway,with a half-wave potential of 0.8 V versus RHE,while the Ni-HAT-CN catalyze ORR in a 2e^(-)pathway with H_(2)O_(2) selectivity over 90%.Moreover,the Co-HAT-CN delivered an overpotential of 350 mV at 10 mA cm^(-2) with a corresponding Tafel slope of 24 mV dec^(-1) for OER in a 1.0 M KOH aqueous *** experimental results revealed that the activities toward ORR were due to the M-N_(4) sites in the frameworks,and both M-N_(4) and M-N_(2) sites contributed to the *** work gives us a new platform to construct bifunctional catalysts.

关键词： covalent organic frameworks metal organic polymers oxygen evolution reaction oxygen reduction reaction single atom catalysts

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Developments of photo‐/electro‐catalysis based on covalent organic frameworks:A review

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Electron 2024年第4期2卷 72-93页

作者： Guiping Yang Qing Xu Gaofeng Zeng CAS Key Laboratory of Low‐Carbon Conversion Science and Engineering Shanghai Advanced Research Institute(SARI)Chinese Academy of Sciences(CAS)ShanghaiChina School of Chemical Engineering University of Chinese Academy of SciencesBeijingChina

Photo‐/electro‐catalysis has the characteristics of low cost,high perfor-mance,and zero pollution,which meet the policies on environment and *** organic frameworks(COFs),a type of crystalline organic skeleton polymers,have been widely applied and investigated in the area of photo‐/electro‐catalysis owing to their advantages of large specific surface area,regular pore size,excellent stability,flexible structural design,and massive active *** article reviews the structural characteristics of COFs and the strategies for strengthening the photo‐/electro‐catalytic activity of COF ***,deep insights were put into the photo‐/electro‐catalysis application of COF *** the end,the development prospects and challenges faced by COF materials in photo‐/electro‐catalysis are discussed.

关键词： covalent organic frameworks electrocatalysis photocatalysis

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Li-promoted C_(3)N_(4) catalyst for efficient isomerization of glucose into fructose at 50℃ in water

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Green Energy & Environment 2024年第9期9卷 1419-1426页

作者： Wang Liu Yanfei Zhang Mengya Sun Xinpeng Zhao Shenggang Li Xinqing Chen Liangshu Zhong Lingzhao Kong CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai201210China University of Chinese Academy of Sciences Beijing100049China School of Physical Science and Technology Shanghai Tech UniversityShanghai201203China School of Environmental Science and Engineering Suzhou University of Science and TechnologySuzhouJiangsu215009China

Efficient and selective glucose-to-fructose isomerization is a crucial step for production of oxygenated chemicals derived from sugars,which is usually catalyzed by base or Lewis acid heterogeneous ***,high yield and selectivity of fructose cannot be simultaneously obtained under mild conditions which hamper the scale of application compared with enzymatic ***,a Li-promoted C_(3)N_(4) catalyst was exploited which afforded an excellent fructose yield(40.3 wt%)and selectivity(99.5%)from glucose in water at 50℃,attributed to the formation of stable Li–N bond to strengthen the basic sites of ***,the so-formed N_(6)–Li–H_(2)O active site on Li–C_(3)N_(4) catalyst in aqueous phase changes the local electronic structure and strengthens the deprotonation process during glucose isomerization into *** superior catalytic performance which is comparable to biological pathway suggests promising applications of lithium containing heterogeneous catalyst in biomass refinery.

关键词： Glucose Fructose Isomerization Li–C_(3)N_(4) Density functional theory calculations

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Dealuminated Hβ zeolite for selective conversion of fructose to furfural and formic acid

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Green Energy & Environment 2024年第2期9卷 311-320页

作者： Rui Li Qixuan Lin Junli Ren Xiaobao Yang Yingxiong Wang Lingzhao Kong State Key Laboratory of Pulp and Paper Engineering School of Light Industry and EngineeringSouth China University of TechnologyGuangzhou510640China Institute of Coal Chemistry Chinese Academy of Sciences27 South Taoyuan RoadTaiyuan030001China CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai201210China School of Environmental Science and Technology Suzhou University of Science and Technology Suzhou Jiangsu215009China

The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at433 K for 1 h in the γ-butyrolactone(GBL)-H_(2)O system, as well as the concomitant formation of 83.0% formic acid. The^(13)C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.

关键词： Fructose Dealuminated-Hb zeolite Selective conversion Furfural

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Nickel-modified In_(2)O_(3) with inherent oxygen vacancies for CO_(2) hydrogenation to methanol

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science China Chemistry 2024年第5期67卷 1715-1728页

作者： Zixuan Zhou Yuchen Wang Yuanjie Bao Haiyan Yang Jiong Li Chunran Chang Shenggang Li Peng Gao CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization School of Chemistry and Chemical EngineeringYulin UniversityYulin 719000China

Methanol synthesis is one of the most important industrially-viable approaches for carbon dioxide(CO_(2)) utilization, as the produced methanol can be used as a platform chemical for manufacturing green fuels and chemicals. The In_(2)O_(3) catalysts are ideal for sustainable methanol synthesis and have received considerable attention. Herein, Co-, Ni-and Cu-modified In_(2)O_(3) catalysts were fabricated with high dispersion and high stability to improve the hydrogenation performance. The Ni-promoted In_(2)O_(3) catalyst in the form of high dispersion possessed the largest amount of oxygen vacancies and the strongest ability for H_(2) activation, leading to the highest CO_(2) conversion and space time yield of methanol of 0.390 g_(Me OH)g_(cat)^(-1)h^(-1) with CH_(3)OH selectivity of 68.7%. In addition, the catalyst exhibits very stable performance over 120 h on stream, which suggests the promising prospect for industrial applications. Further experimental and theoretical studies demonstrate that surface Ni doping promotes the formation of oxygen defects on the In_(2)O_(3) catalyst, although it also results in lower methanol selectivity. Surprisingly, subsurface Ni dopants are found to be more beneficial for methanol formation than surface Ni dopants, so the Nipromoted In_(2)O_(3)catalyst with a lower surface Ni content at the similar Ni loading can reach higher methanol selectivity and productivity. This work thus provides theoretical guidance for significantly improving the CO_(2) reactivity of In_(2)O_(3)-based catalysts while maintaining high methanol selectivity.

关键词： carbon dioxide hydrogenation methanol synthesis indium oxides Ni doping sites transition metal promoters

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Diatomic Pd catalyst with conjugated backbone for synergistic electrochemical CO_(2)reduction

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Nano Research 2024年第6期17卷 4850-4855页

作者： Wenxuan Zhang Mengran Zhang Hongjuan Wang Wen Zhang Min Zhang MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion School of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China

Double-site catalysts have attracted widespread attention in the field of electrocatalysis due to their high metal loading,adjustable active centres,and electronic valence ***,the development of bimetallic sites catalysts that coordinate with definite atoms is still in the exploratory ***,we designed and synthesized a bimetallic palladium complex(BPB-Pd_(2))with conjugated *** supported BPB-Pd_(2)was applied to electrochemical CO_(2)reduction reaction(CO_(2)RR)for the first *** as-obtained BPB-Pd_(2)gives an exceptional Faradaic efficiency of CO(FECO)of 94.4%at−0.80 V *** hydrogen electrode(RHE),which is significantly superior to monoatomic palladium catalyst(BPB-Pd1).The density functional theory(DFT)calculations revealed that the essential reason for the outstanding activity of BPB-Pd_(2)toward CO_(2)RR was that the electronic effect between diatomic palladium reduces the free energy change for CO_(2)RR ***,BPB-Pd_(2)exhibits moderate free energy change to form COOH*intermediate,which was beneficial for the generation of CO in CO_(2)RR.

关键词： synthesis electrocatalysis CO_(2)reduction bimetallic palladium complex synergistic catalysis

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Strong interaction between Fe and Ti compositions for effective CO_(2)hydrogenation to light olefins

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Chinese Journal of Catalysis 2025年第4期71卷 146-157页

作者： Hao Liang Shunan Zhang Ruonan Zhang Haozhi Zhou Lin Xia Yuhan Sun Hui Wang Institute of Carbon Neutrality ShanghaiTech UniversityShanghai 201203China CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China

Fe-based catalysts are widely used for CO_(2)hydrogenation to light olefins(C_(2–4)=);however,precise regulation of active phases and the balance between intermediate reactions remain significant ***,we find that the addition of moderate amounts of Ti forms a strong interaction with Fe compositions,modulating the Fe_(3)O_(4)and Fe_(5)C_(2)*** interaction leads to an increased Fe_(5)C_(2)/Fe_(3)O_(4)ratio,which in turn enhances the adsorption of reactants and intermediates,promoting CO hydrogenation to unsaturated alkyl groups and facilitating C–C ***,the strong Fe-Ti interaction induces the preferential growth of Fe_(5)C_(2)into prismatic structures that expose the(020),(–112),and(311)facets,forming compact active interfacial sites with Fe_(3)O_(4)*** facet and interfacial effects significantly promote the synergistic coupling of the reverse water gas shift and Fischer-Tropsch *** optimized 3K/FeTi catalyst with the highest Fe_(5)C_(2)/Fe_(3)O_(4)ratio of 3.6 achieves a 52.2%CO_(2)conversion rate,with 44.5%selectivity for C2–4=and 9.5%for CO,and the highest space-time yield of 412.0 mg gcat^(–1)h^(–1)for C_(2–4)=.

关键词： CO_(2)hydrogenation Light olefins Strong Fe-Ti interaction Fe_(5)C_(2) Active phase modulation

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Dimensional engineering of covalent organic frameworks derived carbons for electrocatalytic carbon dioxide reduction

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SusMat 2023年第6期3卷 834-842页

作者： Guojuan Liu Xuewen Li Minghao Liu Xiubei Yang Zhuangyan Guo Xinqing Chen Qing Xu Gaofeng Zeng Yue He CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute(SARI)Chinese Academy of Sciences(CAS)ShanghaiChina School of Chemical Engineering University of Chinese Academy of SciencesBeijingChina Shanghai Ninth People’s Hospital Shanghai Jiao Tong UniversityShanghaiChina

Covalent organic frameworks(COFs)have been developed as the precursors to construct porous carbons for electrocatalytic ***,the influences of carbon dimensions on the catalytic performance are still *** this work,we have first constructed COF-derived carbons by template-synthesis strategy in different dimensions to catalyze the carbon dioxide reduction(CO_(2)RR).By using different templates,the one-dimensional(1D),two-dimensional(2D),and three-dimensional(3D)COF-derived carbons have been employed to anchor Co-porphyrin to form the Co-N5 sites to catalyze CO_(2)*** 1D catalyst templated by carbon nano tubes presents high binding ability of CO_(2),more defective sites,and higher electronic conductivity,resulting in a higher catalytic activity for CO_(2)and selectivity of CO than 2D and 3D carbon-based *** 1D catalyst delivers the turnover frequency values of 1150 h^(−1)and the FECO of 94.5%at 0.7 V versus RHE,which is significantly better than those of 2D and 3D carbon-based catalysts.

关键词： CO_(2)reduction Co-N_(5)sites covalent organic frameworks dimensional engineering templatesynthesis strategy

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