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A post-modification strategy to precisely construct dual-atom sites for oxygen reduction electrocatalysis

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Journal of Energy Chemistry 2024年第3期90卷 511-517,I0012页

作者： Juan Wang Xinyan Liu Chang-Xin Zhao Yun-Wei Song Jia-Ning Liu Xi-Yao Li Chen-Xi Bi Xin Wan Jianglan Shui hong-jie peng Bo-Quan Li Jia-Qi Huang School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina School of Materials Science and Engineering Beihang UniversityBeijing 100191China

Dual-atom catalysts(DACs) afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic ***,precise construction of dual-atom sites remains a *** this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction ***,a secondary metal precursor is introduced to the primary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construction of *** as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0,91 V *** hydrogen ***-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C *** importantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom *** work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices.

关键词： Dual-atom catalysts Electrocatalysis Oxygen reduction reaction Post-modification Zinc–air batteries

Encapsulating-polysulfide electrolyte: An answer to practical lithium-sulfur batteries

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Chinese Chemical Letters 2023年第3期34卷 3-4页

作者： hong-Li Long hong-jie peng Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731China

Endowed with high theoretical specific energy(2600 Wh/kg) and low material cost, lithium-sulfur(Li-S) battery emerges as a promising candidate for the next-generation energy storage system. A working Li-S battery is in fact a liquid electrochemical system where the reaction of solid S/lithium sulfide(Li_(2)S) proceeds via dissolved lithium polysulfides(LiPSs) intermediates [1].

关键词： battery lithium sulfide

Review of nanostructured current collectors in lithium-sulfur batteries

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Nano Research 2017年第12期10卷 4027-4054页

作者： Long Kong hong-jie peng Jia-Qi Huang Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Beijing 100084 China

Lithium-sulfur （Li-S） batteries are receiving increasing attention because of their high theoretical energy density and the natural abundance of S. However, their practical applications are impeded by the low areal S loading in the cathode and the fatal Li dendrites in the anode of the Li-S cells, which yield an inferior practical energy density and introduce safety concerns, respectively. In this review, we focus on an emerging approach--the nanostructured current collector--to overcome these two critical challenges for Li-S batteries. We describe the general attributes of nanostructured current collectors and examine how these attributes enhance the S utilization with a high S loading and suppress the Li dendrites by regulating the Li-deposition behavior. We present various assembly blocks that have been used for the construction of advanced nanostructured current collectors to build better S cathodes and Li anodes. Finally, we investigate the current challenges and possible solutions regarding the practical applications of nanostructured current collectors in Li-S batteries.

关键词： Li-S batteries nanostructured currentcollectors Li metal anode graphene C nanotubes composite cathode

A perspective on the electrocatalytic conversion of carbon dioxide to methanol with metallomacrocyclic catalysts

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Journal of Energy Chemistry 2022年第1期31卷 263-275,I0008页

作者： Xinyan Liu Bo-Quan Li Bing Ni Lei Wang hong-jie peng Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina 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 Physical Chemistry Department of ChemistryUniversity of KonstanzUniversitatsstrasse 10D-78457 KonstanzGermany Department of Chemical and Biomolecular Engineering National University of Singapore.Singapore 117585Singapore

Electrocatalytic carb on dioxide reducti on(CO_(2)R)presents a promising route to establish zero-e mission carb on cycle and store in termittent ren ewable energy into chemical fuels for steady energy *** is an ideal energy carrier as alternative fuels and one of the most important commodity ***,methanol is currently mainly produced from fossil-based syngas,the production of which yields tremendous carb on emission *** CO_(2)R towards metha nol poses great potential to shift the paradigm of methanol *** this perspective,we focus our discussions on producing methanol from electrochemical CO_(2)R,using metallomacrocyclic molecules as the model *** discuss the motivation of having methanol as the sole CO_(2)R product,the documented application of metallomacrocyclic catalysts for CO_(2)R,and recent advance in catalyzing CO_(2) to methanol with cobalt phthalocyanine-based *** attempt to understand the key factors in determining the activity,selectivity,and stability of electrocatalytic CO_(2)-to-methanol conversion,and to draw mechanistic insights from existing ***,we identify the challenges hindering methanol electrosynthesis directly from CO_(2) and some intriguing directions worthy of further investigation and exploration.

关键词： Carbon dioxide reduction Methanol Electrocatalysis Molecular catalysts Single atom catalysts Heterogenization

New insights into “dead lithium” during stripping in lithium metal batteries

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Journal of Energy Chemistry 2021年第11期30卷 289-294,I0007页

作者： Xiao-Ru Chen Chong Yan Jun-Fan Ding hong-jie peng Qjang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084 China Advanced Research Institute of Multidisciplinary Science School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081 China Department of Chemical Engineering Stanford UniversityStanfordCA 94305USA

Lithium (Li) metal attributes to the promising anode but endures the low Columbic efficiency (CE) and safety issues from the inactive Li accumulation. The metallic Li which is isolated from the lithium anode (named dead Li^(0)) consists the major component of the inactive Li. We systematically and meticulously investigated the formation and evaluation of dead Li^(0) during stripping process from electron transfer, the oxidation of Li^(0) to Li^(+) and the diffusion of Li^(+) through solid electrolyte interphase (SEI). The above-mentioned processes were regulated by adjusting the contact sites of electron channels, the dynamic rate of conversion from Li^(0) to Li^(+), and the structure as well as components of SEI. The design principles for achieving less dead Li^(0) and higher CE are proposed as a proof of concept in lithium metal batteries. This new insight sheds a comprehensive light on dead Li^(0) formation and guides the next-generation safe batteries for future application.

关键词： Lithium metal batteries Dead lithium Lithium stripping Lithium dendrite growth Charge transfer

Metal/nanocarbon layer current collectors enhanced energy efficiency in lithium-sulfur batteries

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Science Bulletin 2017年第18期62卷 1267-1274页

作者： Jia-Qi Huang Pei-Yan Zhai hong-jie peng Wan-Cheng Zhu 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 Department of Chemical Engineering Qufu Normal University

Lithium-sulfur （Li-S） batteries with intrinsic merits in high theoretical energy density are the most promising candidate as the next-generation power sources. The strategy to achieve a high utilization of active materials with high energy efficiency is strongly requested for practical applications with less energy loss during repeated cycling. In this contribution, a metal/nanocarbon layer current collector is proposed to enhance the redox reactions of polysulfides in a working Li-S cell. Such a concept is demon- strated by coating graphene-carbon nanotube hybrids （GNHs） on routine aluminum （AI） foil current collectors. The interracial conductivity and adhesion between the current collector and active material are significantly enhanced. Such novel cell configuration with metal/nanocarbon layer current collectors affords abundant Li ions for rapid redox reactions with small overpotential. Consequently, the Li-S cells with nanostructured current collectors exhibit an initial discharge capacity of 1,113 mAh g-1 at 0.5 C, which is -300 mAh g-1 higher than those without a GNH coating layer. The capacity retention is 73% for cells with GNH after 300 cycles. A reduced voltage hysteresis and a high energy efficiency of ca. 90% are therefore achieved. Moreover, the AI/GNH layer current collectors are easily implanted into current cell assembly process for energy storage devices based on complex multi-electron redox reactions （e.g., Li-S batteries, Li-O2 batteries, fuel cells, and flow batteries）.

关键词： Lithium-sulfur battery Nanostructured current collectors Polysulfides Energy efficiency Pouch cell

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

Sodiophilicity/potassiophilicity chemistry in sodium/potassium metal anodes

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Journal of Energy Chemistry 2020年第12期29卷 1-6页

作者： Xiang Chen Yun-Ke Bai Xin Shen hong-jie peng Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Department of Chemical Engineering Stanford UniversityStanfordCA 94305USA

Heteroatom-doped carbon materials have been widely used as sodium(Na) and potassium(K) metal anode frameworks to achieve uniform Na and K depositions. If the origin of the Sodiophilicity and potassiophilicity of doping sites in heteroatom-doped carbon host are clearly understood, the nucleation and growth behavior of Na and K can be precisely regulated in working batteries. Herein the Sodiophilicity and potassiophilicity chemistries of carbon materials are probed through first-principles calculations. The local dipole of doping functional groups and charge transfer during Na/K deposition are regarded as key principles to reveal the sodiophilic and potassiophilic nature of doping sites. Especially, O–B, O–S, and O–P co-doping strategy are predicted to be effective methods to improve the Sodiophilicity and potassiophilicity of carbon hosts and thus render safe and dendrite-free Na and K metal anodes. This work affords a deep and insightful understanding of Sodiophilicity and potassiophilicity chemistry of Na and K anodes and establishes general principles of designing highly sodiophilic and potassiophilic carbon frameworks.

关键词： Sodium and potassium metal anodes Sodiophilicity and potassiophilicity Carbon materials First-principles calculations Dendrite-free electrode

A two-dimension laminar composite protective layer for dendrite-free lithium metal anode

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Journal of Energy Chemistry 2021年第5期30卷 391-394页

作者： Xiang-Qun Xu Rui Xu Xin-Bing Cheng Ye Xiao hong-jie peng hong Yuan Fangyang Liu School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina 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 Department of Chemical Engineering Stanford UniversityStanfordCA 94305 USA

Lithium(Li)metal anodes with the high theoretical specific capacity(3860 mAh g^(-1))and most negative reduction potential(-3.04 V *** hydrogen electrode)have been considered as an ultimate choice for energy storage devices with high energy density[1-4].However,the practical applications of Li metalbased batteries(LMBs)are confronted with two tough issues:Li dendrite growth induced by uneven Li depositions and unstable solid electrolyte interphase(SEI)(Fig.1a)[5,6].

关键词： Lithium metal anode Artificial protective layer 2D materials Vermiculite sheets Laminar arrangement