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Selective oxygen electroreduction to hydrogen peroxide in acidic media:The superiority of single-atom catalysts

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Nano Research 2024年第6期17卷 4668-4681页

作者： Ergui Luo Tongtong Yang Jingyi Liang Yuhong Chang Junming Zhang Tianjun Hu Junjie Ge Jianfeng Jia key laboratory of Magnetic Molecules and Magnetic Information materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China School of Chemistry and materials Science University of Science and Technology of ChinaHefei 230026China State key laboratory of Electroanalytic Chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Two-electron oxygen reduction reaction(2e-ORR)provides an environmentally friendly direction for the on-site production of hydrogen peroxide(H_(2)O_(2)).Central to this technology is the exploitation of efficient,economical,and safe 2e-ORR *** overview starts with the fundamental chemistry of ORR to highlight the decisive role of adsorbing intermediates on the reaction pathway and activity,followed by a comprehensive survey of the tuning strategies to favor 2e-ORR on traditional precious *** latest achievements in designing efficient and selective precious-metal-based single-atom catalysts(SACs)and metal-nitrogen-carbon(M-Nx/C)catalysts,from the aspects of material synthesis,theoretical calculations,and mass transport promotion,are systematically *** introductions on the evaluation metrics for 2e-ORR catalysts and the primary reactor designs for cathodic H_(2)O_(2)synthesis are also *** conclude this review with an outlook on the challenges and direction of efforts to advance electrocatalytic 2e-ORR into realistic H_(2)O_(2)production.

关键词： oxygen reduction reaction H_(2)O_(2)production single-atom catalysts selectivity

Engineering S-scheme W_(18)O_(49)/ZnIn_(2)S_(4)heterojunction by Co_(x)P nanoclusters for enhanced charge transfer capability and solar hydrogen evolution

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Nano Research 2024年第9期17卷 8095-8103页

作者： Xiaojie Liu Erkang Liu Zixian Wang Wen Zhang Mingyu Dou Hua Yang Changhua An Dacheng Li Jianmin Dou Shandong Provincial key laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252059China Tianjin key laboratory of Organic Solar Cell and Photochemical conversion School of Chemistry and Chemical EngineeringTianjin Key Laboratory of Advanced Functional Porous MaterialsInstitute for New Energy Materials and Low-Carbon TechnologiesTianjin University of TechnologyTianjin 300384China Institute of Powder Metallurgy and Advanced Ceramics School of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China

Enhancement of the light-absorption response and utilization of the photogenerated carriers represent a robust strategy for the design of high-performance *** this work,grafting Co_(x)P nanoclusters onto S-scheme heterojunction of W18O49/ZnIn2S4(WO/ZIS-CoxP)with strong response to the ultraviolet-visible-near infrared ray(UV-vis-NIR)region has been achieved,which possesses efficient electron-transfer-channel,and boosts charge-separation and transport *** as-prepared WO/ZIS-Co_(x)P yields an impressive solar-driven hydrogen production rate of 45 mmol·g^(-1)·h^(-1).The increased photocatalytic performance is attributed to the synergistic effect of the composite catalyst:(1)The local surface plasmon resonance-induced“hot electron”injection of W_(18)O_(49)significantly increases the electron density;(2)the engineered S-scheme directional electron transfer promotes charge separation and enhances the reducing capability of photoexcited electrons;and(3)Co_(x)P as electron-trap site for accelerating surface proton reduction *** work provides a platform to impart nonprecious co-catalyst for engineering S-scheme heterojunction,serving a class of efficient solar-driven photocatalyst towards hydrogen production.

关键词： hydrogen cocatalyst photocatalysis S-scheme hot electron

Grading of products utilizing bamboo as a substitute for plastic based on environmental effects

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Science China Earth Sciences 2024年第9期67卷 2989-2998页

作者： Meng ZHANG Guomo ZHOU Lei GU Wenshuo WANG College of Forestry Beijing Forestry UniversityBeijing 100083China key laboratory of carbon Cycling in Forest Ecosystems and carbon Sequestration of Zhejiang province Zhejiang A&F UniversityHangzhou 311300China

To achieve sustainable development goals,mitigate plastic pollution,and promote eco-friendly products,it is crucial to identify key products in the bamboo as a substitute for plastic(BSP)industry and assess their environmental *** study proposed a novel evaluation method for the environmental effect of bamboo as a substitute for plastic(EBSP).It focused on the contributions of BSP products in reducing plastic pollution and greenhouse gas *** established a set of EBSP evaluation indicators and developed a grading model,evaluating 30 typical BSP products across six *** results showed that the EBSP evaluation model,based on the emission reduction rate of substitution(ERRS),substitution rate of material(SRM),and product renewal ratio(PRR),can accurately quantify the environmental benefits of BSP *** model has successfully facilitated precise quantification of the EBSP and established a rational and effective grading system for BSP *** results also demonstrated that the average EBSP ranking across the six categories of BSP products,in descending order,is:disposable bamboo products,bamboo household goods,bamboo packaging products,bamboo engineering materials,bamboo furniture products,and bamboo craft ***,disposable bamboo products scored an EBSP 1.96 times the overall average,indicating significant environmental *** PRR emerged as a critical factor influencing *** BSP products with the same lifespan,those with higher substitution emission reduction efficiency offered more pronounced environmental ***,the BSP industry should strategically prioritize disposable bamboo products,such as bamboo toothbrushes,cutlery,and lunch *** products should be the primary focus of policy support and central to efforts in product development,design innovation,and market promotion.

关键词： Bamboo as a substitute for plastic Bamboo products Substitution emission reduction Environmental benefits Gradingevaluation

Discovery and intensity characterization of TDP and PRP based on temperature evolution history during the pyrolysis for large biomass particle

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carbon Resources conversion 2024年第3期7卷 41-50页

作者： Rui Chen Jun Cai Xinli Li Xiaobin Qi State key laboratory of coal conversion Institute of Engineering ThermophysicsChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences No.19 Yuquan RoadShijingshan DistrictBeijing 100049China Shanxi Engineering Research Center of coal Clean Efficient Combustion and GasificationNo.1619 Yunzhou StreetDatong CityShanxi Province 037305China Shanxi key laboratory of coal Flexible Combustion and Thermal conversion No.1619 Yunzhou StreetDatong CityShanxi Province 037305China

The pyrolysis behaviors and temperature evolution history of lignocellulosic biomass(Beech,BH)were characterized using a novel pyrolysis *** simulation results were validated through corresponding experimental *** on the simulation results,two distinct peaks were observed in the temperature difference between the surface and center(TDSC)curve,namely the thermal disturbance peak(TDP)and the pyrolysis reaction peak(PRP).The presence of TDP and PRP was confirmed by examining the heat flux ratio between the pyrolysis rate and the temperature rise ***,the results indicated that three factors,namely heating temperature,particle size,and pyrolysis rate,influenced the relative intensity between TDP and *** changing the values of each impact factor,conditions where TDP owns the same height with PRP were obtained under different working *** findings have led to the development of a dimensionless number,naming the pyrolysis-heating surface-center number(PHSC number).This number could provide a comprehensive indication of the collective impact of the aforementioned factors when TDP and PRP exhibit equal peak heights.

关键词： DAEM Large biomass particle Pyrolysis Temperature distribution Dimensionless number

Performance of iron-air battery with iron nanoparticle-encapsulated C-N composite electrode

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Frontiers in Energy 2024年第1期18卷 42-53页

作者： Can FANG Xiangmei TANG Jiaoyan WANG Qingfeng YI School of Chemistry and Chemical Engineering Hunan University of Science and TechnologyXiangtan 411201China Hunan Provincial key laboratory of Advanced materials for new Energy Storage and conversion Xiangtan 411201China

Highly efficient and stable iron electrodes are of great significant to the development of iron-air battery(IAB).In this paper,iron nanoparticle-encapsulated C–N composite(NanoFe@CN)was synthesized by pyrolysis using polyaniline as the C–N *** performance of the NanoFe@CN in different electrolytes(alkaline,neutral,and quasi-neutral)was investigated via cyclic voltammetry(CV).The IAB was assembled with NanoFe@CN as the anode and IrO_(2)+Pt/C as the *** effects of different discharging/charging current densities and electrolytes on the battery performance were also *** K_(2)SO_(4)electrolyte can effectively suppress the passivation of iron electrode,and the battery showed a good cycling stability during 180 charging/discharging *** to the pure nano-iron(NanoFe)battery,the NanoFe@CN battery has a more stable cycling stability either in KOH or NH_(4)Cl+KCl electrolyte.

关键词： energy storage and conversion metallic composites nanocomposites iron-air battery iron anode

Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

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Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang key laboratory of Catalysis and Energy materials Chemistry of Ministry of Education&hubei key laboratory of Catalysis and materials Science South-Central Minzu UniversityWuhan 430074China hubei key laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique *** structural sensitivity of these catalysts is closely linked to their particle size and crystal ***,comprehending the structure–activity relationship requires the development of well-defined Co-based ***,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon *** nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO *** adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal *** influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been *** result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 ***,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(carbon *** findings demonstrate the importance of particle size in Co catalyzed Fischer–Tropsch *** use of well-defined CoO/CS catalysts offers valuable insights into the structure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

Recent advances and practical challenges of high-energy-density flexible lithium-ion batteries

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Frontiers of Chemical Science and Engineering 2024年第8期18卷 79-98页

作者： Guangxiang Zhang Xin Chen Yulin Ma Hua Huo Pengjian Zuo Geping Yin Yunzhi Gao Chuankai Fu State key laboratory of Space Power-Sources Harbin Institute of TechnologyHarbin 150001China MIIT key laboratory of Critical materials Technology for new Energy conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

With the rapid iteration and update of wearable flexible devices,high-energy-density flexible lithium-ion batteries are rapidly ***,energy density,and safety are all important indicators for flexible lithium-ion batteries,which can be determined jointly by material selection and structural ***,recent progress on high-energy-density electrode materials and flexible structure designs are *** electrode materials and the next-generation high-energy-density electrode materials are analyzed in *** electrolytes with high safety and excellent flexibility are classified and *** strategies to increase the mass loading of active materials on the electrodes by designing the current collector and electrode structure are discussed with keys of representative *** the novel configuration structures to enhance the flexibility of batteries are *** the end,it is pointed out that it is necessary to quantify the comprehensive performance of flexible lithium-ion batteries and simultaneously enhance the energy density,flexibility,and safety of batteries for the development of the next-generation high-energy-density flexible lithium-ion batteries.

关键词： lithium-ion batteries flexibility high energy density safety

Dual-functional POM@IL complex modulate hole transport layer properties and interfacial charge dynamics for highly efficient and stable perovskite solar cells

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Chinese Chemical Letters 2024年第7期35卷 461-464页

作者： Boyuan Hu Jian Zhang Yulin Yang Yayu Dong Jiaqi Wang Wei Wang Kaifeng Lin Debin Xia MIIT key laboratory of Critical materials Technology for new Energy conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

The severe interfacial charge recombination as well as the stability issues brought by the Li-TFSI still hinder the commercialization of high-performance perovskite solar cells(PSCs).Here,a polyoxometalates(POMs)-based complex,POM@ionic liquid(IL),is synthesized and applied as an effective additive that simultaneously enhances the performance and stability of *** interactions between POM@IL complex and Li-TFSI inhibit the aggregation of *** synergistic oxidation of POM@IL complex and Li-TFSI towards 2,2,7,7-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene(Spiro-OMeTAD)effectively enhances the electrical properties of hole transport layer film and the photovoltaic performances of *** champion device modified with the POM@IL complex yields an excellent power conversion efficiency(PCE)of 22.73%.Moreover,the incorporation of POM@IL improves the humidity stability of *** storing under high humidity conditions(25℃,60%RH)for 1200 h,the POM@IL modified device retained a remarkable 81.2%of its initial *** work provides new insight into constructing POMs-based materials for high-performance photovoltaic devices.

关键词： Polyoxometalates Ionic liquid Perovskite solar cells Energy alignment Humidity stability

A DFT study on Pt single atom loaded COF for efficient photocatalytic CO_(2)reduction

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Journal of materials Science & Technology 2024年第3期170卷 87-94页

作者： Fei Xie Chuanbiao Bie Jian Sun Zhenyi Zhang Bicheng Zhu laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan430078China key laboratory of new Energy and Rare Earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials and Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Minzu UniversityDalian116600China

Photocatalytic CO_(2)reduction provides a promising strategy for the alleviation of greenhouse effect and energy shortage *** single atom modification is an effective method to improve the CO_(2)reduction performance of covalent organic framework(COF)photocatalysts,while the intrinsic mechanism is not revealed in ***,a Pt-COF photocatalytic system was constructed by embedding Pt single atom in TFPT-TMT-COF(TFPT:1,3,5-tris(4-formylphenyl)-triazine,TMT:2,4,6-trimethyl-1,3,5-triazine).Based on density functional theory(DFT)calculation,the geometric structure and electronic property of Pt-COF were investigated,and the CO_(2)adsorption and reduction reaction process on Pt-COF were *** results show that the Pt atom can be steadily anchored in COF via the formation of Pt-N and Pt-C ***,there is strong electronic interaction between Pt and *** incorporation of Pt atom benefits the CO_(2)reduction activity of COF from multiple aspects:(ⅰ)reducing the band gap and improving light absorption;(ⅱ)enhancing CO_(2)adsorption and activating the CO_(2)molecule;(ⅲ)decreasing the energy barrier in the hydrogenation step of CO_(2)→COOH,thus facilitating CO_(2)conversion to CO;(ⅳ)inhibiting the hydrogenation of CO,thereby increasing the selectivity of *** work brings a novel insight into the excellent CO_(2)reduction performance of Pt modified COF,and provides useful references for the design of single atom photocatalysts.

关键词： Photocatalysis carbon dioxide reduction Covalent organic framework Pt single atom Theoretical calculation