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Tandem Co–O dual sites on halloysite with promoted reaction kinetics for sulfur reduction

Journal of Energy Chemistry 2022年第12期75卷 486-493,I0013页

作者： Qiang Zhang Yinyin Qian Ji-Jun Zou Ruijie Gao huaming yang Engineering Research Center of Nano-Geomaterials of Ministry of Education China University of GeosciencesWuhan 430074HubeiChina Hunan Key Laboratory of Mineral Materials and Application School of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083HunanChina Faculty of Materials Science and Chemistry China University of GeosciencesWuhan 430074HubeiChina Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Key Laboratory of Functional Geomaterials in China Nonmetallic Minerals Industry China University of GeosciencesWuhan 430074HubeiChina

Facilitating sulfur reduction reaction(SRR)is a promising pathway to tackle the polysulfide shuttle effect and enhance the electrochemical performance of lithium-sulfur(Li-S)batteries.Catalysts with a solo active site can reduce a reaction barrier of a certain transition-intermediate,but the linear scaling relationship between multi-intermediates still obstructs overall SRR.Herein,we construct tandem Co–O dual sites with accelerating SRR kinetics by loading highly dispersed cobalt sulfide clusters on halloysite.This catalyst features Co with upshifted d-orbital and O with downshifted p-orbital,which cooperatively adsorb long-chain polysulfide and dissociate an S–S bond,thus achieving both optimal adsorption–desorption strength and reduced conversion energy barrier of multi-intermediates in SRR.The Li-S coin batteries using the electrocatalyst endows a high specific capacity of 1224.3 m Ah g^(-1)at 0.2 C after 200cycles,and enhances cycling stability with a low-capacity decay rate of 0.03%per cycle at 1 C after1000 cycles.Moreover,the strategy of the tandem Co–O dual sites is further verified in a practical Li-S pouch battery that realizes 1014.1 m Ah g^(-1)for 100 cycles,which opens up a novel avenue for designing electrocatalysts to accelerate multi-step reactions.

关键词： Sulfur reduction reaction Dual catalytic site Orbit Li-S battery

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Efficient anion immobilization enabled by structurally controllable halloysite for dendrite-free sodium metal anode

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中国科学:化学英文版 2023年第9期66卷 2600-2611页

作者： Caihong yang Yicheng Hua Ying Zhang Jie Wang Huanwen Wang Liangjie Fu Aidong Tang huaming yang Engineering Research Center of Nano-Geomaterials of Ministry of Education China University of GeosciencesWuhan 430074China Laboratory of Advanced Mineral Materials China University of GeosciencesWuhan 430074China Faculty of Materials Science and Chemistry China University of GeosciencesWuhan 430074China College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Hunan Key Laboratory of Mineral Materials and Application School of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083China

Sodium metal has shown great potential as an inexpensive anode for rechargeable batteries. However, the growth of sodium dendrites continues to hinder the commercialization of Na metal batteries. Herein, an effective strategy using anion-anchoring halloysite nanotube(HNT) coating was proven to prevent the diffusion of anions and trigger uniform Na deposition. Through theoretical calculation, a model of active site of fixed anions exposed from HNTs after acid activation was established for the first time, revealing that Si–Al sites are effective active site of acid-activated HNTs. Furthermore, HNTs with strong and effective adsorption capacity for anions were obtained by controlling the structure of HNTs to regulate the exposure of Si–Al sites. The strong interaction between sites of acid-activated HNTs and the SO_(3)CF_(3)^(-) anion effectively promotes the dissociation of sodium salts, the release of Na^(+) and subsequent migration. As a result, HNTs acid activation for 4 h shows a steady sodium deposition process and displays high Coulombic efficiency in half cell, long cycle life in symmetric cell and full cell. This work provides a basic theoretical basis for the design of nanoclay with abundant and effective active site to fix anions for dendritic free metal batteries.

关键词： halloysite anion immobilization ion transport sodium dendrites sodium metal batteries

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Upcycling of phosphogypsum waste for efficient zinc-ion batteries

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Journal of Energy Chemistry 2023年第6期81卷 157-166,I0006页

作者： Huanwen Wang Can Luo Yinyin Qian Caihong yang Xiaojun Shi Yansheng Gong Rui Wang Beibei He Jun Jin Aidong Tang Edison Huixiang Ang huaming yang Engineering Research Center of Nano-Geomaterials of Ministry of Education China University of GeosciencesWuhan 430074HubeiChina Faculty of Materials Science and Chemistry China University of GeosciencesWuhan 430074HubeiChina Key Laboratory of Functional Geomaterials in China Nonmetallic Minerals Industry China University of GeosciencesWuhan 430074HubeiChina College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083HunanChina Natural Sciences and Science Education National Institute of EducationNanyang Technological UniversitySingapore 637616Singapore School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083HunanChina

Zinc metal is a promising anode material for next-generation aqueous batteries,but its practical application is limited by the formation of zinc dendrite.To prevent zinc dendrite growth,various Zn^(2+)-conducting but water-isolating solid-electrolyte interphase(SEI)films have been developed,however,the required high-purity chemical materials are extremely expensive.In this work,phosphogypsum(PG),an industrial byproduct produced from the phosphoric acid industry,is employed as a multifunctional protective layer to navigate uniform zinc deposition.Theoretical and experimental results demonstrate that PG-derived CaSO_(4)2H_(2)O can act as an artificial SEI layer to provide fast channels for Zn^(2+)transport.Moreover,CaSO_(4)2H_(2)O could release calcium ions(Ca^(2+))due to its relatively high Kspvalue,which have a higher binding energy than that of Zn^(2+)on the Zn surface,thus preferentially adsorbing to the tips of the protuberances to force zinc ions to nucleate at inert region.As a result,the Zn@PG anode achieves a high Coulombic efficiency of 99.5%during 500 cycles and long-time stability over 1000 hours at 1 m A cm^(-2).Our findings will not only construct a low-cost artificial SEI film for practical metal batteries,but also achieve a high-value utilization of phosphogypsum waste.

关键词： Upcycling Phosphogypsum waste Zinc-ion battery Solid-electrolyte-interface Protection layer

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Aqueous Zn-based rechargeable batteries:Recent progress and future perspectives

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InfoMat 2022年第5期4卷 67-101页

作者： Mingjie Wu Gaixia Zhang huaming yang Xianhu Liu Marc Dubois Marc AGauthier Shuhui Sun Institut National de la Recherche Scientifique(INRS)-CentreEnergie Matériaux Télécommunications VarennesQuébecCanada Engineering Research Center of Nano-Geomaterials of Ministry of Education China University of GeosciencesWuhanChina Department of Inorganic Materials School of Minerals Processing and BioengineeringCentral South UniversityChangshaChina Key Laboratory of Materials Processing and Mold Ministry of EducationZhengzhou UniversityZhengzhouChina UniversitéClermont Auvergne CNRSSIGMA ClermontInstitut de Chimie de Clermont-FerrandClermont-FerrandFrance

Benefiting from the advantageous features of high safety,abundant reserves,low cost,and high energy density,aqueous Zn-based rechargeable batteries(AZBs)have received extensive attention as promising candidates for energy storage.To achieve high-performance AZBs with high reversibility and energy density,great efforts have been devoted to overcoming their drawbacks by focusing on the modification of electrode materials and electrolytes.Based on different cathode materials and aqueous electrolytes,the development of aqueous AZBs with different redox mechanisms are discussed in this review,including insertion/extraction chemistries(e.g.,Zn^(2+),alkali metal ion,H^(+),NH_(4)^(+),and so forth dissolution/deposition reactions(e.g.,MnO_(2)/Mn^(2+)),redox couples in flow batteries(e.g.,I_(3)/3I,Br_(2)/Br,and so forth),oxygen electrochemistry(e.g.,O_(2)/OH,O_(2)/O_(2)2),and carbon dioxide electrochemistry(e.g.,CO_(2)/CO,CO_(2)/HCOOH).In particular,the basic reaction mechanisms,issues with the Zn electrode,aqueous electrolytes,and cathode materials as well as their design strategies are systematically reviewed.Finally,the remaining challenges faced by AZBs are summarized,and perspectives for further investigations are proposed.

关键词： aqueous Zn-based rechargeable batteries hybrid battery Zn–air battery Zn–CO_(2)battery Zn-ion battery

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Engineering a tubular mesoporous silica nanocontainer with well-preserved clay shell from natural halloysite

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Nano Research 2017年第8期10卷 2782-2799页

作者： Liangjie Fu huaming yang Aidong Tang Yuehua Hu Centre for Mineral Materials School of Minerals Processing and Bioengineering Central South University Changsha 410083 China Peter A. Rock Thermochemistry Laboratory and NEATORU University of California Davis One Shields Avenue Davis CA 95616 USA Hunan Key Lab of Mineral Materials & Application Central South University Changsha 410083 China School of Chemistry and Chemical Engineering Central South University Changsha 410083 China

The in situ synthesis of mesoporous nanotubes from natural minerals remains a great challenge. Herein, we report the successful synthesis of mesoporous silica nanotubes （MNTs） with a varying inner-shell thickness and a preserved clay outer shell from natural-halloysite nanotubes （HNTs）. After the enlargement of the lumen diameter of the tubular aluminosilicate clay by acid leaching, uniform mesopores were introduced by a modified pseudomorphic transformation approach, while the clay outer shell was well-preserved. Using density functional theory calculations, the atomic structure evolution and the energetics during A1 leaching and Si-OH condensation were studied in detail. After the leaching of A1 ions from the HNTs, local structural changes from Al（Oh） to A1（V） at a medium leaching level and to AI（Td） at a high leaching level were confirmed. The calculated hydroxylation energy of two kinds of silica components in the acid-leached HNTs （the distorted two-dimensional silica source in the inner shell and the intact aluminosilicate structure in the outer shell） was 0.5 eV lower or 1.0 eV higher than that of bulk silica, which clarifies the different behavior of the silica components in the hydrothermal process. The successful synthesis of reactive MNTs from HNTs introduces a new strategy for the synthesis of mesoporous nanocontainers with a special morphology using natural minerals. In particular, MNT samples with numerous reactive AI（V） species and a specific surface area up to 583 m^2/g （increased by a factor of 10） are promising drugloading nanocontainers and nanoreactors.

关键词： halloysite mesoporous nanotubes acid leaching hydrothermal synthesis density functional theory （DFT） calculation nanocontainer

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Hierarchical MoS2 intercalated clay hybrid nanosheets with enhanced catalytic activity

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Nano Research 2017年第2期10卷 570-583页

作者： Kang Peng Liangjie Fu huaming yang Jing Ouyang Aidong Tang Centre for Mineral Materials School of Minerals Processing and Bioengineering Central South University Changsha 410083 China Hunan Key Lab of Mineral Materials & Application Central South University Changsha 410083 China State Key Lab of Powder Metallurgy Central South University Changsha 410083 China School of Chemistry and Chemical Engineering Central South University Changsha 410083 China

Emerging hierarchical MoS2/pillared-montmorillonite （MoS2/PMMT） hybrid nanosheets were successfully prepared through facile in-situ hydrothermal synthesis of MoS2 within the interlayer of cetyltrimethylammonium bromide PMMT, and their catalytic performance was evaluated by the reduction reaction of 4-nitrophenol （4-NP） using NaBH4 as a reductant. Microstructure and morphology characterization indicated that MoS2/PMMT exhibited hybrid-stacked layered structures with an interlayer spacing of 1.29 nm, and the MoS2 nanosheets were intercalated within the montmorillonite （MMT） layers, with most of the edges exposed to the outside. The catalytic activity and stability of MoS2/PMMT were both enhanced by the MMT. With the MoS2/PMMT as the catalyst, the apparent reaction rate constant of the 4-NP reduction was 0.723 min-1 and was maintained at -0.679 min-1 after five reaction cycles. The structural evolution of MoSdPMMT and the possible catalysis mechanism for the reduction reaction of 4-NP were investigated. The as-prepared MOSR/PMMT hybrid nanosheets are promising candidates for catalytic application in the water-treatment and biomedical fields. The strategy developed in this study can provide insights for designing hybrid nanosheets with diverse heterogeneous two-dimensional （2D） nanomaterials.

关键词： pillared montmorillonite,MoS2,hybrid nanosheets,hydrothermal synthesis,heterogeneous catalysis

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Intercalated kaolinite as an emerging platform for cancer therapy

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Science China Chemistry 2019年第1期62卷 58-61页

作者： Yi Zhang Peng Huang Mei Long Song Liu huaming yang Shuwen Yuan Shi Chang Department of Inorganic Materials School of Minerals Processing and Bioengineering Central South University Hunan Key Laboratory of Mineral Materials and Application Central South University Xiangya Hospital Central South University Institute of Chemical Biology and Nanomedicine College of Chemistry and Chemical Engineering Hunan University Department of Radiology The Second Xiangya Hospital Central South University

An innovative cancer therapy strategy regarding the interface engineering of kaolinite has been designed. The exposed silanol group facilitates more guest species with high dispersion on the supports. Mn_3O_4 magnetic nanoparticles are uniformly distributed on external surfaces of the Kaolin_(C12N)with the Al–O–Mn bond for the detection of the tumor microenvironment by T1-MRI; Doxorubicin(DOX) are loaded in the interlayer space with the electrostatic interaction for chemo-treating; and KI is coated on the outer layer of the nanocomposites based on the electrostatic interaction for thyroid cancer targeting. The synergetic effects and the treatment mechanism enhanced by the interface engineering, KI@DOX-Mn_3O_4-Kaolin_(C12N)can cause remarkably low cell viability(57%, 200 μg/mL), tumor shrinking(75%, 20 μg/kg), and accumulation into the tumor tissues. The novel kaolinite based drug delivery system is expected to incorporate imaging diagnosis, targeted therapy and drug delivery into one single system for postoperative residual thyroid cancer treatment and observation for metastasis of focal area.

关键词： kaolinite pillared drug delivery system thyroid cancer

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Net energy,energy utilization,and nitrogen and energy balance affected by dietary pea supplementation in broilers

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Animal Nutrition 2021年第2期7卷 506-511页

作者： Nishchal K.Sharma Zhibin Ban Hank L.Classen huaming yang Xiaogang Yan Mingan Choct Shu-Biao Wu School of Environmental and Rural Science University of New EnglandArmidaleNSW 2351Australia Laboratory of Animal Nutrition Metabolism Jilin Academy of Agricultural SciencesGongzhulingJilin 136100China Department of Animal and Poultry Science University of Saskatchewan51 Campus DriveSaskatoonSK S7N 5A8Canada Office of the Pro Vice-Chancellor External Relations University of New EnglandArmidaleNSW 2351Australia

Pea starch consists predominantly of C-type of amylopectin chain which is more resistant to digestive enzymes than A-type of starch thus slowly digested in poultry.It was hypothesized that the presence of slowly digested pea starch in broiler diets will increase net energy and the efficiency of energy utilization in broilers.Two experiments were performed to investigate starch digestibility of pea at different in-cubation times(in vitro study)and the effect of dietary pea on heat increment and net energy in broilers using an open-circuit respiratory calorimetry system(in vivo study).One-day-old Ross 308 male broilers were fed a common starter crumble from d 1 to 10 and standard grower diets thereafter.At d 21,birds were transferred to the chambers each housing 2 birds.Each treatment was replicated 6 times with 2 identical runs of 3 replicates per treatment.A wheat-soybean meal-based diet was used as a control and the treatment diet contained 500 g of pea/kg pea.In vitro study showed that pellet processing increased(P0.05)FCR compared to those offered the wheat-based *** energy(NE)and apparent metabolizable energy(AME)values were higher in the pea-based diet than in the wheat-based diet(P-0.037 for NE and P-0.018 for AME).Heat production,respiratory quotient,heat increment of feed,efficiency of utilization of gross energy for AME,and efficiency of utilization of AME for NE did not differ(P>0.05)between the 2 treatments.There was no effect(P>0.05)of pea on the total tract di-gestibilities of dry matter,crude protein and ash,but the total tract digestibility of starch was higher(P-0.022)in the pea-based diet compared to the wheat-based diet.This study provides insight into the energy metabolism of broilers offered a pea-based diet and indicates that dietary pea supplementation increases dietary AME and NE b

关键词： Slowly digested starch Pea Heat increment Net energy Broiler

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Intercalated 2D nanoclay for emerging drug delivery in cancer therapy

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Nano Research 2017年第8期10卷 2633-2643页

作者： Yi Zhang Mei Long Peng Huang huaming yang Shi Chang Yuehua Hu Aidong Tang Linfeng Mao Department of Inorganic Materials School of Minerals Processing and Bioengineering Central South University Changsha 410083 China Xiangya Hospital Central South University Changsha 410078 China Hunan Key Laboratory of Mineral Materials and Application Central South University Changsha 410083 China School of Chemistry and Chemical Engineering Central South University Changsha 410083 China

Natural two-dimensional （2D） kaolinite nanoclay has been incorporated into an emerging drug delivery system. The basal spacing of the kaolinite nanoclay was expanded from 0.72 to 4.16 nm through the intercalation of various organic guest species of different chain lengths, which can increase the efficiency in drug delivery and reduce the toxicity of doxorubicin （DOX）. Original kaolinite （Kaolin） and the Kaolin intercalation compounds exhibited a high level of biocompatibility and very low toxicity towards cells of pancreatic cancer, gastric cancer, prostate cancer, breast cancer, colorectal cancer, esophageal cancer, and differentiated thyroid cancer. However, lung cancer and hepatocellular cancer cells need more strict compositional, structural, and morphological modulations for drug delivery carriers. DOX-Kaolin and the DOX-Kaolin intercalation compounds showed dramatically faster drug release in moderately acidic solution than in neutral condition, and exhibited enhanced therapeutic effects against ten model cancer cell cultures in a dose-dependent manner. The use of 2D nanoclay materials for a novel drug delivery system could feasibly pave a way towards high-performance nanotherapeutics, with superior antitumor efficacy and significantly reduced side effects.

关键词： cancer therapy nanoclay intercalation drug delivery biocompatibility

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碳纳米纤维调控粉煤灰基地质聚合物力学/传感性能优化

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中南大学学报（自然科学版） 2024年第3期55卷 907-917页

作者：范兴昊刘叶帆张国昊欧阳静杨华明胡海龙张帆中南大学资源加工与生物工程学院湖南长沙410083 中南大学矿物材料及其应用湖南省重点实验室湖南长沙410083 中南大学航空航天技术研究院湖南长沙410083

采用物理混合法向粉煤灰基地质聚合物中加入碳纳米纤维(CNF),制备不同CNF质量分数(0~2.0%)的粉煤灰基地质聚合物复合材料。通过对粉煤灰基地质聚合物复合材料微结构、力学性能、电学性能及传感性能进行研究,揭示CNF调控粉煤灰基地质聚... 详细信息

采用物理混合法向粉煤灰基地质聚合物中加入碳纳米纤维(CNF),制备不同CNF质量分数(0~2.0%)的粉煤灰基地质聚合物复合材料。通过对粉煤灰基地质聚合物复合材料微结构、力学性能、电学性能及传感性能进行研究,揭示CNF调控粉煤灰基地质聚合物力学与传感性能的具体演变规律,并对CNF质量分数为0.5%的复合材料进行循环稳定性实验及方差稳定性量化分析。研究结果表明:当CNF添加量增加时,粉煤灰基地质聚合物的弹性模量和抗弯强度皆显著提升;当CNF质量分数为0.5%和2.0%时,复合材料的弹性模量分别提升到1.35 MPa和0.23 MPa,抗弯强度分别提升到3.9 MPa和0.32 MPa;此外,随CNF质量分数增加,复合材料的电阻率随之降低,当CNF质量分数达到2.0%时,复合材料的电阻率降低到46Ω·m,CNF的添加有利于粉煤灰基地质聚合物导电能力提升;在单向加压实验条件下,当CNF质量分数为0.5%、1.0%和2.0%时,复合材料的传感灵敏度分别为71.56、57.33与25.58,随着CNF的加入量不断增大,粉煤灰基地质聚合物的传感灵敏度先增后减,通过实验判断CNF质量分数阈值可能为0~0.5%。在CNF质量分数为0.5%的条件下,复合材料传感性能相对比较稳定。

关键词：地质聚合物碳纳米纤维传感性能健康监测

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