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Crafting Pyrolysis-Free M−N−C Catalysts

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Precision Chemistry 2023年第5期1卷 264-271页

作者： chang-xin zhao Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

M−N−C catalysts,with their transition metal atoms coordinated to nitrogen/carbon atoms as active sites,are gaining attention for their versatile heterogeneous *** of these catalysts can be achieved through either bottom-up chemical synthesis or top-down pyrolysis procedures,where the former offers a well-defined structure and precise synthesis *** Perspective provides an overview of the history of the technical route dispute between pyrolysis and pyrolysis-free M−N−C catalysts,along with their respective advantages and ***,we emphasize the advantages of pyrolysis-free M−N−C catalysts,exemplified by several studies focused on precisely modulating the structure to regulate the activity,as well as the efforts of effectively integrating the active ***,we discuss the challenges and opportunities of pyrolysis-free M−N−C catalysts,with the aim of maximizing their inherent strengths of precise structure and promoting their industrial applications.

关键词： M−N−C catalysts electrocatalysis porphyrin phthalocyanine organic frameworks

Favorable Lithium Nucleation on Lithiophilic Framework Porphyrin for Dendrite-Free Lithium Metal Anodes

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Research 2019年第1期2019卷 1249-1259页

作者： Bo-Quan Li Xiao-Ru Chen Xiang Chen chang-xin zhao Rui Zhang xin-Bing Cheng Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Lithium metal constitutes promising anode materials but sufers from dendrite *** host materials are highly considered for achieving uniform lithium *** construction of lithiophilic sites with desired structure and homogeneous distribution signifcantly promotes the lithiophilicity of lithium hosts but remains a great *** this contribution,a framework porphyrin(POF)material with precisely constructed lithiophilic sites in regard to chemical structure and geometric position is employed as the lithium host to address the above issues for dendrite-free lithium metal *** extraordinary lithiophilicity of POF even beyond lithium nuclei validated by DFT simulations and lithium nucleation overpotentials afords a novel mechanism of favorable lithium nucleation to facilitate uniform nucleation and inhibit dendrite ***,POF-based anodes demonstrate superior electrochemical performances with high Coulombic efciency over 98%,reduced average voltage hysteresis,and excellent stability for 300 cycles at 1.0 mA cm^(−2),1.0 mAh cm^(−2) superior to both Cu and graphene *** favorable lithium nucleation mechanism on POF materials inspires further investigation of lithiophilic electrochemistry and development of lithium metal batteries.

关键词： lithium POF hysteresis

The formation of crystalline lithium sulfide on electrocatalytic surfaces in lithium-sulfur batteries

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Journal of Energy Chemistry 2022年第1期31卷 568-573,I0015页

作者： Yun-Wei Song Jin-Lei Qin chang-xin zhao Meng zhao Li-Peng Hou Yan-Qi Peng Hong-Jie Peng Bo-Quan Li Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengduSichuan 611731China

Lithium-sulfur(Li-S)battery is highly regarded as a promising next-generation energy storage device but suffers from sluggish sulfur redox *** the behavior and mechanism of the sulfur species on electrocatalytic surface is the first step to rationally introduce polysulfide electrocatalysts for kinetic promotion in a working ***,crystalline lithium sulfide(Li_(2)S)is exclusively observed on electrocatalytic surface with uniform spherical morphology while Li_(2)S on non-electrocatalytic surface is amorphous and *** characterization indicates the crystalline Li_(2)S preferentially participates in the discharge/charge process to render reduced interfacial resistance,high sulfur utilization,and activated sulfur redox ***,crystalline Li_(2)S is proposed with thermodynamic and kinetic advantages to rati on alize the superior performances of Li-S *** evoluti on of solid Li_(2)S on electrocatalytic surface not only addresses the polysulfide electrocatalysis strategy,but also inspires further investigation into the chemistry of energy-related processes.

关键词： Lithium-sulfur batteries Polysulfide electrocatalysis Lithium sulfide Framework porphyrin Sulfur redox reactions

Transition metal coordinated framework porphyrin for electrocatalytic oxygen reduction

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Chinese Chemical Letters 2019年第4期30卷 911-914页

作者： chang-xin zhao Bo-Quan Li Jia-Ning Liu Jia-Qi Huang Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology

Oxygen reduction reaction(ORR) constitutes the core process of many clean and sustainable energy systems including fuel cells and metal–air batteries. Developing high-performance and cost-efficiency ORR electrocatalysts is of great significance to the practical applications of the above-mentioned energy storage devices. Transition metal coordinated porphyrin electrocatalysts are highly considered as a promising substitution of noble-metal-based electrocatalyst because of their high ORR reactivity, where the ORR performances of the porphyrin-based electrocatalysts are highly dependent on the transition metal center. Herein a series of framework porphyrin electrocatalysts coordinated with different transition metal centers(M-POF, where M is Mn, Fe, Co, Ni, Cu, or Zn) was designed, synthesized, and evaluated in regards of electrocatalytic ORR performances. Among all, the Co-POF electrocatalyst exhibits the best ORR performances with the highest half-wave potential of 0.81 V vs. RHE and the lowest Tafel slope of 53 mV/dec. This contribution affords an optimized high-performance ORR electrocatalyst and provides instructions for further rational design of porphyrin-based ORR electrocatalysts for sustainable energy applications.

关键词： Electrocatalysis Oxygen reduction reaction Transition metal coordination Framework porphyrin Fuel cells

Regeneration of single-atom catalysts deactivated under acid oxygen reduction reaction conditions

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Journal of Energy Chemistry 2022年第10期31卷 478-484,I0012页

作者： chang-xin zhao Ding Ren Juan Wang Jia-Ning Liu Cheng Tang Xiao Chen Bo-Quan Li Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia

Single-atom catalysts serve as a promising candidate to realize noble-metal-free electrocatalytic oxygen reduction in acid ***,their poor stability under working conditions strictly restrains their practical ***,regeneration of their electrocatalytic activity is of great ***,the regeneration of a Fe-N-C single-atom catalyst is demonstrated to be feasible by a facile annealing regeneration *** activity after regeneration recovers to that of the pristine electrocatalyst and surpasses the deactivated *** regeneration mechanism is identified to be selfetching of the surface carbon layer and consequent exposure of the previously buried single-atom ***,the regeneration strategy is applicable to other single-atom *** work demonstrates the feasibility of regenerating oxygen reduction electrocatalysts and affords a pioneering approach to deal with rapid deactivation under working conditions.

关键词： Oxygen reduction reaction Single-atom catalysts Energy electrocatalysis Noble metal free Catalyst regeneration

Seawater-based electrolyte for Zinc–air batteries

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Green Chemical Engineering 2020年第2期1卷 117-123页

作者： Jia Yu chang-xin zhao Jia-Ning Liu Bo-Quan Li Cheng Tang Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing100081China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA5005Australia

Aqueous zinc–air batteries(ZABs)are highly regarded as a promising electrochemical energy storage device owing to high energy density,low cost,and intrinsic *** employment of seawater to replace the currently used deionized water in electrolyte will bring great economic benefits and broaden the application occasions of ***,ZABs using seawater-based electrolyte remain uninvestigated without an applicable cathode electrocatalyst or a successful battery ***,seawater-based electrolyte is successfully employed in ZABs with satisfactory *** influence of chloride anions on the cathode electrocatalytic reactivity and battery performance is systemically *** noble-metal-based and noble-metal-free electrocatalysts are applicable to the chloride-containing alkaline *** evaluation of ZABs with seawaterbased electrolyte demonstrates comparable battery performances with the conventional electrolyte in terms of polarization,capacity,and rate *** study demonstrates a successful prototype of seawater-based ZABs and enlightens the utilization of natural resources for clean and sustainable energy storag.

关键词： Zinc-air batteries Seawater-based electrolytes Oxygen reduction reaction Electrocatalysis

Composing atomic transition metal sites for high-performance bifunctional oxygen electrocatalysis in rechargeable zinc-air batteries

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Particuology 2023年第6期77卷 146-152页

作者： Juan Wang chang-xin zhao Jia-Ning Liu Ding Ren xinzhi Ma Bo-Quan Li Jia-Qi Huang Qiang Zhan School of Materials Science and Engineering Beijing Institute of TechnologyBeijing100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing100084China Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin150025China

Rechargeable zinc-air batteries have attracted extensive attention as clean,safe,and high-efficient en-ergy storage ***,the oxygen redox reactions at cathode are highly sluggish in kinetics and severely limit the actual battery *** transition metal sites demonstrate high electro-catalytic activity towards respective oxygen reduction and evolution,while high bifunctional electro-catalytic activity is seldomly *** a strategy of composing atomic transition metal sites is proposed to fabricate high active bifunctional oxygen electrocatalysts and high-performance recharge-able zinc-air ***,atomic Fe and Ni sites are composed based on their respective high electrocatalytic activity on oxygen reduction and *** composite electrocatalyst demonstrates high bifunctional electrocatalytic activity(ΔE=0.72 V)and exceeds noble-metal-based Pt/C+Ir/C(ΔE=0.79 V).Accordingly,rechargeable zinc-air batteries with the composite electrocatalyst realize over 100 stable cycles at 25 mA *** work affords an effective strategy to fabricate bifunctional oxygen electrocatalysts for high-performance rechargeable zinc-air batteries.

关键词： Rechargeable zinc-air batteries Bifunctional oxygen electrocatalysis Noble-metal-free electrocatalysts Oxygen reduction reaction Oxygen evolution reaction

Quantitative kinetic analysis on oxygen reduction reaction:A perspective

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Nano Materials Science 2021年第3期3卷 313-318页

作者： Juan Wang chang-xin zhao Jia-Ning Liu Ding Ren Bo-Quan Li Jia-Qi Huang Qiang Zhang School of Materials Science and Engineering Beijing Institute of TechnologyBeijing100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Oxygen reduction reaction(ORR)constitutes the core process of many energy storage and conversion devices including metal–air batteries and fuel ***,the kinetics of ORR is very sluggish and thus highperformance ORR electrocatalysts are highly *** recent progress on minimizing the ORR halfwave potential as the current evaluation indicator,in-depth quantitative kinetic analysis on overall ORR electrocatalytic performance remains insufficiently *** this paper,a quantitative kinetic analysis method is proposed to afford decoupled kinetic information from linear sweep voltammetry profiles on the basis of the Koutecky–Levich *** parameters regarding exchange current density,electron transfer number,and electrochemical active surface area can be respectively determined following the proposed *** quantitative kinetic analysis method is expected to promote understanding of the electrocatalytic effect and point out further optimization direction for ORR electrocatalysis.

关键词： Oxygen reduction reaction Electrocatalysis Quantitative kinetic analysis Koutecky–Levich equation Mass transfer

Multianion Transition Metal Compounds:Synthesis,Regulation,and Electrocatalytic Applications

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Accounts of Materials Research 2021年第11期2卷 1082-1092页

作者： chang-xin zhao Hao-Fan Wang Bo-Quan Li Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory(ChEM-OIL) National Institute of Advanced Industrial Science and Technology(AIST)Kyoto 606-8501Japan Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China

CONSPECTUS:Energy electrocatalysis is an essential part for the modern energy network serving as the core technique in many electrochemical energy devices such as batteries,fuel cells,electrolyzers,*** high-performance electrocatalysts,especially the pursuit for higher intrinsic electrocatalytic activity,is the eternal theme for high-efficiency energy *** metal compounds are highly considered as promising highperformance electrocatalysts due to their facile fabrication,well-defined structure,and encouraging intrinsic ***,further promotion on intrinsic electrocatalytic activity of conventional transition metal compounds encounters an unavoidable bottleneck originated from the rigid homoanion structure with limited choice of *** the above issue,heteroanion substitution on pristine transition metal compounds has been proposed in some recent *** unique structure and properties that distinguish them from routine transition metal compounds have attracted wide attention to reveal distinct electronic structures,synthesis methodologies,and functions in energy electrocatalysis for future application.

关键词： anion Transition intrinsic