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Tuning the atomic configuration environment of MnN_(4) sites by Co cooperation for efficient oxygen reduction

Journal of Energy Chemistry 2023年第7期82卷 547-559,I0012页

作者： Jing Wang Haihong Zhong Jun Yang Huiyu Li Pinggui Tang Yongjun Feng Dianqing Li State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China College of Science Hainan UniversityHaikou 570228HainanChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Carbon-based N-coordinated Mn(Mn-N_(x)/C)single-atom electrocatalysts are considered as one of the most desirable non-precious oxygen reduction reaction(ORR)candidates due to their insignificant Fenton reactivity,high abundance,and intriguing electrocatalytic performance.However,current MnN_(x)/C single-atom electrocatalysts suffer from high overpotentials because of their low intrinsic activity and unsatisfactory chemical stability.Herein,through an in-situ polymerization-assisted pyrolysis,the Co as a second metal is introduced into the Mn-N_(x)/C system to construct Co,Mn-N_(x)dual-metallic sites,which atomically disperse in N-doped 1D carbon nanorods,denoted as Co,Mn-N/CNR and hereafter.Using electron microscopy and X-ray absorption spectroscopy(XAS)techniques,we verify the uniform dispersion of CoN4and MnN4atomic sites and confirm the effect of Co doping on the MnN_(4) electronic structure.Density functional theory(DFT)calculations further elucidate that the energy barrier of ratedetermining step(^(*)OH desorption)decreases over the 2 N-bridged MnCoN_(6) moieties related to the pure MnN_(4).This work provides an effective strategy to modulate the local coordination environment and electronic structure of MnN_(4) active sites for improving their ORR activity and stability.

关键词： Dual-atom sites Oxygen reduction reaction M-Nx/C catalysts Coordination environment Electronic structure Synergistic effect

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Bifunctional oxygen electrode cobalt–nickel sulfides catalysts originated from intercalated LDH precursors

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Journal of Energy Chemistry 2022年第11期31卷 376-386,I0010页

作者： Xiaofei Gong Haihong Zhong Luis Alberto Estudillo-Wong Nicolas Alonso-Vante Yongjun Feng Dianqing Li State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China Departamento de Sociedad y Política Ambiental CIIEMADInstituto Politécnico NacionalCalle 30 de junio de 1520Alcaldía GAMC.P.07340 CDMXMexico IC2MP UMR-CNRS 7285University of PoitiersF-86073 Poitiers CedexFrance

Bimetallic cobalt-nickel sulfide nanoparticles anchored on S-,N-codoped holey carbon nanosheets(CoNiS-T@NCFs)with a hydrangea-like morphology,were synthesized via a confinement synthesis route,in which an intercalated LDH precursor was subjected to the interlayer-confined carbonization and host-layer sulfurization.The phase transformation and structure evolution(e.g.,atom site occupancy,crystallite size,and cell volume)of the CoNi-S-T@NCFs electrocatalysts,as a function of sulfurization temperatures,were confirmed by X-ray diffraction and Rietveld analyses.The sulfur vacancies effectively enhance the electrocatalytic activity,while the synergistic effect of(Co,Ni)7 S8 alloy and S,N-codoped carbon matrix facilitates the electron transfer and accelerates reaction kinetics,making CoNi-S-900@NCFs an efficient and stable bifunctional electrocatalyst for oxygen reduction reaction(ORR).The rich highvalence Co(Ⅲ)and Ni(Ⅲ)of CoNi-S-900@NCFs facilitates the in-situ transformation of the metal(oxy)hydroxides intermediates with high catalytic activity for oxygen evolution reaction(OER).Thus,with a bifunctional parameter,ΔE,of 0.75 V(E_(j=10,OER)-E_(1/2,ORR)),this electrocatalyst slightly outperforms the state-of-the-art commercial Pt/C+RuO_(2)/C catalyst(ΔE=0.76 V)in alkaline medium.This work demonstrates the influence that the sulfurization temperature has on the relationship between the structure and electrocatalytic performance of bimetallic sulfides prepared by the synthesis strategy using the intercalated LDH precursor.This strategy can be extended to prepare other chalcogenides with binary or ternary transition metals.

关键词： Bimetallic sulfides Confinement synthesis LDHs ORR OER

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Oxygen vacancies engineering by coordinating oxygen-buffering CeO_(2) with CoO_(x) nanorods as efficient bifunctional oxygen electrode electrocatalyst

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Journal of Energy Chemistry 2021年第8期30卷 615-625,I0013页

作者： Haihong Zhong Luis Alberto Estudillo-Wong Yuan Gao Yongjun Feng Nicolas Alonso-Vante State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsCollege of ChemistryBeijing University of Chemical TechnologyNo.15 Beisanhuan East Road100029 BeijingChina IC2MP UMR-CNRS 7285University of PoitiersF-86022 Poitiers CedexFrance Departamento de Sociedad y Política Ambiental CIIEMADInstituto Politécnico NacionalCalle 30 de junio de 1520Alcaldía GAMC.P.07340 CDMXMexico Anqing Research Institute Beijing University of Chemical TechnologyNo.8 Huanhu West RoadHigh-Tech DistrictAnqing 24600China

CeO_(2)decorated CoOx rod-like hybrid,supported onto holey reduced graphene(CoOx/CeO_(2)/RGO)composite,was fabricated via a surfactant-assisted route.Its corresponding electrocatalytic performance towards oxygen reduction/evolution reactions(ORR and OER)was systematically investigated in alkaline electrolyte.Structural,morphological and compositional studies revealed changes in electronic and surface properties when CeO_(2)was introduced as an oxygen buffer material.The oxygen vacancies effectively enhanced the electrocatalytic activity,while the synergistic effect of co-catalyst CeO_(2),CoOx activecenters,and defective graphene with many voids facilitate the charge/mass transfer,making CoOx/CeO_(2)/RGO an efficient and stable bifunctional electrocatalyst for OER/ORR with△E=0.76 V(△E=E10mAcm.-2OER-E_(1/2).ORR).This parameter is 70 mV and 270 mV lower than CoOx/RGO and the benchmark Pt/C,respectively.In addition,the OER/ORR bifunctionality of CoOx/CeO_(2)/RGO composite outperforms that of Pt/C catalyst in a H2-O_(2)micro fuel cell platform.

关键词： Co3O4 CeO_(2) Oxygen vacancies ORR OER

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Thermoelectric generator based on anisotropic wood aerogel for low-grade heat energy harvesting

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Journal of Materials Science & Technology 2022年第25期120卷 150-158页

作者： Xuan Zhao Zehong Chen Hao Zhuo Yijie Hu Ge Shi Bing Wang haihong Lai Sherif Araby Wenjia Han Xinwen Peng Linxin zhong State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510641China Department of Mechanical and Aerospace Engineering Nazarbayev University53 Kabanbay Batyr AvenueNur-SultanKazakhstan State Key Laboratory of Bio-based Material and Green Papermaking Qilu University of TechnologyJinan 250353China

Thermoelectric generators(TEGs)have received increasing attention due to their potential to harvest low-grade heat energy(<100℃ )and provide power for the Internet of Things(IoT)and wearable electronic devices.Herein,a wood-based ordered framework is used to fabricate carbon nanotube/poly(3,4-ethylenedioxythiophene)(CNT/PEDOT)wood aerogel for TEG.The prepared CNT/PEDOT wood aerogel with an anisotropic structure exhibits a low thermal conductivity of 0.17 W m^(−1)K^(−1)and is advantageous to develop a sufficient temperature gradient.Meanwhile,CNT/PEDOT composites effectively decouple the relationship between the Seebeck coefficient and electrical conductivity by energy filtering effect to enhance thermoelectric(TE)output properties.The vertical TEG assembled by the CNT/PEDOT wood aerogels reveals an output power of 1.5μW and a mass-specific power of 15.48μW g^(−1)at a temperature difference of 39.4 K.Moreover,the layered structure renders high compressibility and fatigue resistance.The anisotropic structure,high mechanical performance,and rapid thermoelectric response,enabling the TEG based on CNT/PEDOT wood aerogel offer opportunities for continuous power supply to low-power electronic devices.

关键词： Wood Nano cellulose Energy harvesting Wearable devices Thermoelectric generator

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Unraveling specific role of carbon matrix over Pd/quasi-Ce-MOF facilitating toluene enhanced degradation

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Journal of Rare Earths 2022年第11期40卷 1751-1762,I0003页

作者： Chunjing Su Zhi Li Mengqi Mao Wenhua Ye Jinping zhong Quanming Ren Hairong Cheng Haomin Huang Mingli Fu Junliang Wu Yun Hu Daiqi Ye haihong Xu School of Environment and Energy South China University of TechnologyGuangzhou 510006China National Engineering Laboratory for VoCs Pollution Control Technology and Equipment(SCUT) Guangzhou 510006China Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control(SCUT) Guangzhou 510o06China Guangdong Conhgin Parovincial Engineering and Technology Research Centre for Environmental Risk Prevention and Emergency Disposal(SCUT)Guangzhou 510006China Appraisal Center for Environment&Engineering Ministry of Ecology and EnvironmentBeijing 100012China

Metal organic frameworks(MOFs)derivatives represented by quasi-MOFs have excellent physical and chemical properties and can be applied for the catalytic combustion of volatile organic compounds(VOCs).In this work,Pd/quasi-Ce-BTC synthesized by simple one-step Npyrolysis was applied to the oxidation of toluene,showing excellent toluene catalytic activity(T_(90)=175℃,30000 mL/(g·h)).Microscopic analyses indicate the formation and interaction of a carbon matrix composite quasi-MOF structure interface.The results show that the amorphous carbon matrix formed during the partial pyrolysis of Ce-BTC significantly improves the adsorption and activation capacity of toluene in the reaction,and constructs a reductive system to maintain high concentrations of Ce^(3+)and Pd^(0),which can facilitate the activation and utilization of oxygen in reaction.Quasi in-situ XPS proves that carbon matrix is indirectly involved in the activation and storage of oxygen,and Pd^(0)is the crucial active site for the activation of oxygen.Stability and water resistance tests display good stability of Pd/quasi-Ce-BTC.This work provides a potential method for designing quasi-MOF catalysts towards VOCs effective abatement.

关键词： Quasi-MOF Toluene oxidation Carbon matrix Metal nanoparticles Oxygen activation ability Rare earths

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Defect reduction to enhance the mechanical strength of nanocellulose carbon aerogel

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Chinese Chemical Letters 2024年第1期35卷 492-498页

作者： haihong Lai Zehong Chen Hao Zhuo Yijie Hu Xuan Zhao Jiwang Yi Hongzhi Zheng Ge Shi Yifan Tong Ling Meng Xinwen Peng Linxin zhong State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510641China Huangpu Hydrogen Energy Innovation Center/Guangzhou Key Laboratory for Clean Energy and Materials School of Chemistry and Chemical EngineeringGuangzhou UniversityGuangzhou 510006China

Carbon aerogels prepared from renewable nano building blocks are rising-star materials and hold great promise in many fields.However,various defects formed during carbonization at high temperature disfavor the stress transfer and thus the fabrication of flexible carbon aerogel from renewable nano building blocks.Herein,a structural defect-reducing strategy is proposed by altering the pyrolysis route of cellulose nanofiber.Inorganic salt that inhibits the generation of tar volatilization during pyrolysis can prevent the formation of various structural defects.Microstructure with fewer defects can reduce stress concentration and remarkably enhance the compressibility of carbon aerogel,thus increasing the maximum stress retention of carbon aerogel.The carbon aerogel also has high stress sensor sensitivity and excellent temperature coefficient of resistance.The structural defect-reducing strategy will pave a new way to fabricate high-strength carbon materials for various fields.

关键词： Biomass Cellulose nanofiber Pyrolysis Renewable Carbon aerogel

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基于RSEI的北京王平煤矿生态环境修复效果评估及预测

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矿业安全与环保 2023年第4期50卷 89-96页

作者：钟安亚孙娟胡春明谷海红中国科学院生态环境研究中心城市与区域生态国家重点实验室北京100085 华北理工大学矿业工程学院河北唐山063210 北京市生态环境评估与投诉中心北京100161

为研究北京王平煤矿生态修复成效,以1990—2021年Landsat遥感影像数据为基础,采用遥感生态指数(remote sensing ecology index,RSEI)对北京王平煤矿区生态修复工程展开效果评估,并结合GM(1,1)模型对研究区生态环境质量进行动态监测、时... 详细信息

为研究北京王平煤矿生态修复成效,以1990—2021年Landsat遥感影像数据为基础,采用遥感生态指数(remote sensing ecology index,RSEI)对北京王平煤矿区生态修复工程展开效果评估,并结合GM(1,1)模型对研究区生态环境质量进行动态监测、时空分析及预测研究,以期为矿山生态修复工程的管理提供参考。结果表明:1990—2021年,王平煤矿生态环境质量呈现出“先降低,后上升”的势态;1990—2001年研究区RSEI等级差与较差的区域集中在东北部与西南部,生态修复工程开展后,王平煤矿生态环境质量逐年得到改善,少量较差区域集中在东北部边界地区;对王平煤矿RSEI进行预测,预计2025年RSEI将达到0.826,研究区生态环境质量将达到“优”级,表明开展矿山生态修复工程效果较显著。

关键词：生态环境王平煤矿遥感生态指数主成分分析 GM(1,1)模型修复效果

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物理大地测量学课程思政元素挖掘

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测绘通报 2022年第S01期 1-4页

作者：汪海洪钟波褚永海邹贤才武汉大学测绘学院湖北武汉430079 地球空间环境与大地测量教育部重点实验室湖北武汉430079

在分析物理大地测量学课程性质、内容和特点的基础上,从培养科学精神、厚植家国情怀和塑造专业精神等角度对课程蕴含的思政元素进行挖掘,为物理大地测量学课程思政建设提供了参考。

关键词：物理大地测量学课程思政测绘课程建设

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心理距离对道德行为判断的影响

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心理学探新 2013年第1期33卷 43-46页

作者：钟毅平陈海洪湖南师范大学教育科学学院长沙410081

该研究以心理距离的两种表现形式(时间距离和社会距离)为自变量,探讨心理距离对道德行为判断的影响。采用两因素完全被试间设计,120名大学生参加实验,自编道德评价问卷(共四个道德事件)。结果发现,时间距离远近和社会距离不同对道德行... 详细信息

该研究以心理距离的两种表现形式(时间距离和社会距离)为自变量,探讨心理距离对道德行为判断的影响。采用两因素完全被试间设计,120名大学生参加实验,自编道德评价问卷(共四个道德事件)。结果发现,时间距离远近和社会距离不同对道德行为评价的影响存在显著性差异。时间距离越远倾向于高评价,时间距离越近倾向于低评价。发生在自己身上倾向于低评价,发生在他人身上倾向于高评价。结果表明,心理距离对道德行为的判断有重要影响。

关键词：心理距离道德行为道德判断解释水平

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生物质组分快速热解联产生物质炭和碳纳米管的研究

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中国造纸 2024年第4期43卷 1-9页

作者：张帅陈泽虹赖海宏赵轩钟林新华南理工大学制浆造纸国家重点实验室广东广州510640

以纤维素、木聚糖和碱木质素为原料,通过快速热解的方法,使热解挥发性组分在泡沫镍催化下形成上层炭,同时固体产物形成残留固体炭(即下层残炭)。纤维素和木聚糖所得上层炭中含有大量的碳纳米管(CNTs),且掺杂有部分石墨片,而碱木质素则... 详细信息

以纤维素、木聚糖和碱木质素为原料,通过快速热解的方法,使热解挥发性组分在泡沫镍催化下形成上层炭,同时固体产物形成残留固体炭(即下层残炭)。纤维素和木聚糖所得上层炭中含有大量的碳纳米管(CNTs),且掺杂有部分石墨片,而碱木质素则难以形成CNTs。其中,纤维素CNTs比木聚糖CNTs含有更多的石墨化碳,并且纤维素CNTs的石墨化程度、比表面积和产率均较高。纤维素残炭和木聚糖残炭则为致密块状结构,石墨化程度低;纤维素残炭的得率更高,因此纤维素整体的利用率比木聚糖高。结果表明,纤维素和木聚糖的热稳定性较低,热解过程可以产生大量的挥发性组分,且大多为小分子,为CNTs的形成提供了较充足的碳源,而碱木质素的热稳定性高,且热解气体产物少,不利于CNTs的形成。

关键词：生物质热解生物质炭化学气相沉积碳纳米管

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