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Modulating the degree of O vacancy defects to achieve selective control of electrochemical CO_(2) reduction products

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Chinese Chemical Letters 2024年第5期35卷 482-486页

作者： Tianbo Jia Lili Wang Zhouhao zhu Baikang zhu Yingtang Zhou Guoxing zhu mingshan zhu Hengcong Tao School of Petrochemical Engineering&Environment Zhejiang Ocean UniversityZhoushan 316022China Department of General Practice First Medical CenterChinese PLA General HospitalBeijing 100853China National&Local Joint Engineering Research Center of Harbor Oil&Gas Storage and Transportation Technology Zhoushan 316022China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China Guangdong Key Laboratory of Environmental Pollution and Health School of EnvironmentJinan UniversityGuangzhou 511443China

Conversion of CO_(2) into high-value products using electrochemical CO_(2) reduction(ECR)technology is an effective way to alleviate global warming and reach carbon *** oxygen vacancies in heterogenous catalysis are generally considered as a powerful method to enhance the performance of ECR by promoting CO_(2) adsorption and ***,the extent of defects in oxygen vacancies-activity relation has rarely been ***,we prepared Cu-Cd bimetallic catalysts with adjustable oxygen defect degree by controlling the amount of cadmium *** transform infrared spectroscopy characterization results reveal that the formation of oxygen vacancies is attributed to the asymmetric stretching of Cu-O by the addition of *** results show that the oxygen defect degree can modulate the selectivity of ECR products.A low degree of oxygen defects(CuO)is generally associated with lower product Faraday efficiency(FE_(C2)/FE_(C1)≈114%),but overabundant oxygen vacancies(CuO_(2.625)-CdO_(0.375))are not entirely favorable to improving ECR activity(FE_(C2)/FE_(C1)≈125%)and single selectivity,while an appropriate degree of oxygen vacancies(CuO_(2.75)-CdO_(0.25))can facilitate the ECR process toward single product selective production(FE_(C2)/FE_(C1)≈296%).The theoretical calculation showed that the O vacancy formed on CuO and the interface between CdO and CuO were conducive to enhancing the formation of ^(*)COOH intermediate and promoting the generation of ethylene *** study provides a new approach and insight into the selective production of single products for future industrial applications of ECR.

关键词： CO_(2) O-vacancies Bimetallic catalysts Copper oxide Cadmium oxide Selective

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Is reactive oxygen species the only way for cancer inhibition over single atom nanomedicine?Autophagy regulation also works

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Chinese Chemical Letters 2024年第6期35卷 474-479页

作者： Yuanyi Zhou Ke Ma Jinfeng Liu Zirun Zheng Bo Hu Yu Meng Zhizhong Li mingshan zhu Postdoctoral Innovation Practice Base The First and Fifth Affiliated Hospital of Jinan UniversityGuangzhou 510632China Guangdong Provincial Key Laboratory of Spine and Spinal Cord Reconstruction The Fifth Affiliated Hospital of Jinan University(Heyuan Shenhe People’s Hospital)Heyuan 517465China School of Environment Jinan UniversityGuangzhou 511443China Department of Nephrology The First Affiliated Hospital of Jinan UniversityGuangzhou 510632China

Exploring the therapeutic effect of single atom catalysts beyond reactive oxygen species(ROS)modulation would boost the prosperity of nanomedicine in cancer *** as a vital therapy target offers new options for the control of renal cell carcinoma(RCC)***,Fe single atom-decorated graphene oxide(Fe_(1)-GO)nanosheet is developed to be a feasible autophagy inducer in RCC *** the well-dispersed O-Fe_(1)-O active sites,Fe_(1)-GO kills ACHN cells effectively but maintains acceptable cytotoxicity to the normal podocyte and HK2 ***-depth analyses ascribe the inhibition of ACHN cells to the upregulated autophagy instead of the commonly known catalytic ROS *** in vivo therapeutic effect of Fe_(1)-GO nanomedicine is also validated by the RCC-bearing BALB/c mice model,realizing an 89% reduction of tumor weight and good *** work provides new insights into the design of autophagy regulators as well as potential therapeutic strategies for RCC treatment.

关键词： Fe single atom Autophagy Renal cell carcinoma Graphene oxide Cancer therapy

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Novel P-doping-tuned Pd nanoflowers/S,N-GQDs photo-electrocatalyst for high-efficient ethylene glycol oxidation

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Chinese Chemical Letters 2024年第6期35卷 541-545页

作者： Xiaoxiao Huang Zhi-Long He Yangpeng Chen Lei Li Zhenyu Yang Chunyang Zhai mingshan zhu School of Materials Science and Chemical Engineering Ningbo UniversityNingbo 315211China College of Biological Chemical Sciences and EngineeringJiaxing UniversityJiaxing 314001China Guangdong Key Lab oratory of Environmental Pollution and Health School of EnvironmentJinan UniversityGuangzhou 510632China

Traditional photo-electcatalyst structures of small noble metal nanoparticles assembling into large-scale photoactive semiconductors still suffer from agglomeration of noble metal nanoparticles,insufficient charge transfer,undesirable photoresponse ability that restricted the photo-electrocatalytic *** this end,a novel design strategy is proposed in this work,namely integrating small-scale photoactive materials(doped graphene quantum dots,S,N-GQDs)with large-sized noble metal(Pd P)nanoflowers to form novel photo-electrocatalysts for high-efficient alcohol oxidation *** expected,superior electrocatalytic performance of Pd P/S,N-GQDs for ethylene glycol oxidation is acquired,thanks to the nanoflower structure with larger specific surface area and abundant active ***,nonmetal P are demonstrated,especially optimizing the adsorption strength,enhancing the interfacial contact,reducing metal agglomeration,ensuring uniform and efficient doping of S,N-GQDs,and ultimately significantly boost the catalytic activity of photo-electrocatalysts.

关键词： Non-metallic P–doping Sulfur nitrogen co-doped graphene quantum dots Pd nanoflowers Photo-electrocatalytic Ethylene glycol oxidation

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单原子活化过一硫酸盐性能更好?与金属氧化物耦合可能更高效

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Chinese Journal of Catalysis 2024年第4期59卷 137-148页

作者：张俊磊刘文聪刘彪段晓光敖志敏朱明山暨南大学环境学院广东省环境污染与健康重点实验室广东广州511443 北京师范大学环境与生态前沿交叉研究院广东珠海519087 阿德莱德大学化工学院澳大利亚阿德莱德西北工业大学材料科学与工程学院凝固技术国家重点实验室陕西西安710072

单原子催化剂(SAC)作为新一代过一硫酸盐(PMS)非均相活化剂,具有原子利用率高、结构稳定性强等优点,为新兴有机污染物(EOPs)的高效降解提供了新的解决方案.然而,SAC的活性位点密度依然受限于严苛的制备工艺等,而这严重影响PMS的进一步激... 详细信息

单原子催化剂(SAC)作为新一代过一硫酸盐(PMS)非均相活化剂,具有原子利用率高、结构稳定性强等优点,为新兴有机污染物(EOPs)的高效降解提供了新的解决方案.然而,SAC的活性位点密度依然受限于严苛的制备工艺等,而这严重影响PMS的进一步激活.因此,发展SAC基PMS高级氧化技术的关键之一在于提升SAC的活性位点密度,进而增强PMS活化效率.相比之下,传统的过渡金属氧化物(MOx)作为PMS活化剂,尽管存在金属原子利用率低和金属离子易溶出等问题,但其表面具有丰富的金属活性位点.统筹SAC与MOx的优缺点,本文提出了一种“新-老”结合策略,即将传统MOx与新一代SAC耦合,发展兼具丰富金属活性位点和优良结构稳定性的PMS活化剂,实现PMS的高效活化.本文采用预配位-重结晶-热解路径,结合金属离子源投加量控制,制备了具有金属氧化物与单原子组分的Co_(3)O_(4)@Co1/C_(3)N_(5)复合PMS非均相活化剂,并系统研究了其活化PMS降解EOPs的性能.粉末X射线衍射、X射线光电子能谱、高角环形暗场扫描透射电子显微镜及X射线吸收谱结果表明,Co_(3)O_(4)@Co1/C_(3)N_(5)由金属氧化物Co_(3)O_(4)和单原子Co1/C_(3)N_(5)组成,并且Co_(3)O_(4)纳米晶体被锚定在Co1/C_(3)N_(5)纳米片表面.在降解典型EOPs双氯芬酸钠(DCF)的过程中,Co_(3)O_(4)@Co1/C_(3)N_(5)活化的PMS体系展现了显著增强的性能.相比基于Co_(3)O_(4)和Co1/C_(3)N_(5)活化的PMS体系,DCF的降解速率分别提高了约28.0倍和2.5倍,证明Co_(3)O_(4)@Co1/C_(3)N_(5)具有显著增强的PMS活化能力.这主要因为Co1/C_(3)N_(5)和Co_(3)O_(4)之间形成的Co1-O(Co_(3)O_(4))和Co-N(Co1/C_(3)N_(5))化学键有效地促进了电荷迁移.结合密度泛函理论计算发现,Co1/C_(3)N_(5)和Co_(3)O_(4)之间的强电子相互作用显著强化了PMS的吸附,降低了PMS分解生成活性物质的能垒.此外,Co_(3)O_(4)@Co1/C_(3)N_(5)具有良好的复杂环境因素(包括pH、共存阴离子以及实际污水等)耐受性和可重复使用性,证明了其在PMS高级氧化体系中的应用潜力.综上,将单原子催化剂与金属氧化物进行耦合,不仅可能优化电子结构,增强活性位点的暴露度,还能通过协同效应,促进反应中间体的稳定和转化,从而提升整体的PMS活化性能.本文研究结果为设计高效催化剂体系提供了参考.

关键词：单原子催化剂金属氧化物协同效应过一硫酸盐活化 Co_(3)O_(4)@Co1/C_(3)N_(5)

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低成本耐高温海水基胍胶压裂液

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钻井液与完井液 2024年第2期41卷 256-261页

作者：宫大军吴志明白岩朱明山王雪稳袁哲中国石油长城钻探工程有限公司昆山公司江苏昆山215300 昆山京昆油田化学科技有限公司江苏昆山215300

海上油气田压裂由于条件限制,采用淡水配制压裂液导致运输成本高、周期长。海水配制压裂液,碱性交联环境螯合剂加量大,材料成本高,耐温能力一般。针对以上情况采用钛酸四异丙酯、硫酸锆等物质作为反应原料,分步合成有机钛锆交联剂。经... 详细信息

海上油气田压裂由于条件限制,采用淡水配制压裂液导致运输成本高、周期长。海水配制压裂液,碱性交联环境螯合剂加量大,材料成本高,耐温能力一般。针对以上情况采用钛酸四异丙酯、硫酸锆等物质作为反应原料,分步合成有机钛锆交联剂。经核磁碳谱、交联剂沉析后扫描电镜表征,表明交联剂为有机螯合物,动静态同步激光光散射仪表征交联剂尺寸,表明交联剂粒子直径主要为1~100 nm,具有良好的反应活性。该交联剂在中性条件下即可交联,适应海水等高矿化度水质配制压裂液,其交联微观形态为蜂窝状六元网格状结构,结构稳定,黏弹性相比单钛交联有明显的提升,耐温能力可达180℃以上。在中海油南海区域施工实验一口海水配液高温井,效果良好。

关键词：高矿化度海水胍胶耐高温低成本

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Efficient ozone decomposition over bifunctional Co_(3)Mn-layered double hydroxide with strong electronic interaction

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Chinese Chemical Letters 2022年第10期33卷 4679-4682页

作者： Bin Liu Minxian Zhang Jingling Yang mingshan zhu Guangdong Key Laboratory of Environmental Pollution and Health School of EnvironmentJinan UniversityGuangzhou 511443China

Ground-level ozone is one of the primary pollutants detrimental to human health and *** ozone decomposition still suffers from low efficiency and unsatisfactory *** this work,we report a manganese-based layered double hydroxide catalyst(Co_(3)Mn-LDH),which exhibited a superior ozone decomposition performance with the efficiency of 100% and stability over 7 h under a GHSV of 2,000,000 mL g^(-1)h^(-1) and relative humidity of 15%.Even when the relative humidity increased to 50%,the ozone decomposition also reached 86%,which significantly exceeds as-synthesized MnO_(2) and commercial MnO_(2) in *** catalytic mechanism was studied by H_(2)-TPR,FT-IR and *** excellent performance of Co_(3)Mn-LDH can be attributed to its abundant surface hydroxyl groups that ensured the preferentially surface enrichment of ozone,as well as the cyclic dynamic replenishment of electrons between multivalent Co^(2+)/Co^(3+),Mn^(2+)/Mn^(3+)/Mn^(4+)and oxygen species that endowed the stable ozone *** work offers new insights into the design of efficient catalysts for ozone pollution control.

关键词： Co_(3)Mn-layered double hydroxide Ozone removal Hydroxyl groups Bifunctional catalysis Heterogeneous catalysis

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Cascaded electron transition proved by femto-second transient absorption spectroscopy for enhanced photocatalysis hydrogen generation

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Chinese Chemical Letters 2023年第4期34卷 363-367页

作者： Xin Wang Huiqian Jiang mingshan zhu Xiaowei Shi Department of Applied Chemistry Zhejiang University of TechnologyHangzhou 310031China School of Environment Jinan UniversityGuangzhou 511443China

Regulating flow direction of photo-excited electrons from interior to active sites in surface is critical to enhance the photocatalytic performance. Herein, photoinduced chemical reduction process was utilized to pinpoint deposit CdS and NiS nanodots sequentially onto g-C_(3)N_(4)nanosheets. The resulted hybrid composite NiS/CdS/g-C_(3)N_(4)was much more active under visible light, and eventually boosted the hydrogen evolution rate of 3015 μmol g^(-1)h^(-1), to be 2.4 folds better than that of g-C_(3)N_(4). Because of the relative low content of CdS(around 3.0 wt%), the enhanced activity is due to the favoring band overlapping and promoting charge separation rather than increasing light absorption. Femto-second time-resolved transient absorption spectroscopy(fs-TAS) clearly reveals that the photo-excited electrons are from g-C_(3)N_(4),and then migrate unidirectionally to CdS and finally to NiS, which is caused by the precisely regulate the position of CdS and NiS on g-C_(3)N_(4)surface. This study elucidates the electron transfer kinetics and processes in multi-component system and affords a new avenue to construct stable photocatalysts with high activity.

关键词： Photocatalysis Hydrogen generation g-C_(3)N_(4) Ternary heterostructure Charge transfer

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Near-infrared response Pt-tipped Au nanorods/g-C_(3)N_(4) realizes photolysis of water to produce hydrogen

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Journal of Materials Science & Technology 2022年第24期119卷 53-60页

作者： Yang Guo Qixin Zhou Xiaolin Chen Yunzhi Fu Shenyu Lan mingshan zhu Yukou Du School of Science Hainan UniversityHaikou570228China School of Environment Jinan UniversityGuangzhou511443China College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China

The search for a suitable cocatalyst for graphitic carbon nitride(g-C_(3)N_(4)) to realize efficient photocatalytic hydrogen(H_(2)) evolution has been regarded as one of the most valid tactics to alleviate energy ***,a ternary Pt-tipped Au nanorods(Pt-Au)/g-C_(3)N_(4) heterostructure is constructed,which shows excellent H_(2) production performance in visible and near-infrared(NIR) region,especially in NIR region with a rate of 51.6 μmol g^(-1)h^(-1).Therein,not only is the optical absorption ability of g-C_(3)N_(4) broadened,the light absorption range is also extended to NIR region through introduction of Pt-Au ***,analysis of the hot electrons generated in energy relaxation of plasmon indicates hot electron transfers fromexcited Au nanorods to Pt nanoparticles,resulting in H_(2) *** with bare g-C_(3)N_(4),the superior photocatalytic activity could be attributed to the surface plasmon resonance effect(SPR) of Au nanorods and the electron-sink function of Pt *** work provides an insight into the improvement of photocatalytic performance via combination of NIR-responsive plasmon metal with photocatalysts.

关键词： Near infrared response Photocatalysis H_(2)evolution g-C_(3)N_(4) Pt-tipped Au nanorods

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Enhanced utilization efficiency of peroxymonosulfate via water vortex-driven piezo-activation for removing organic contaminants from water

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Environmental Science and Ecotechnology 2022年第2期10卷 38-44页

作者： Chuan Yu Jie He Shenyu Lan Wanqian Guo mingshan zhu Guangdong Key Laboratory of Environmental Pollution and Health School of EnvironmentJinan UniversityGuangzhou511443PR China State Key Laboratory of Urban Water Resource and Environment Harbin Institute of TechnologyHarbin150090PR China

The efficient activation and utilization of peroxymonosulfate(PMS)in PMS-based advanced oxidation processes is a high-priority target for the removal of organic *** work introduces a water vortex-driven piezoelectric effect from few-odd-layered MoS_(2)into the PMS activation to remove benzotriazole(BTR)and other organic contaminants from the *** 91.1%of BTR can be removed by the MoS_(2)piezo-activated PMS process with a reaction rate constant of 0.428 min1,which is 2.09 times faster than the sum of the individual MoS_(2),water vortex,and piezocatalysis ***,the PMS utilization efficiency reached 0.0147 in the water vortex-driven piezo-activation system,which is 3.97 times that of the sum from the vortex/PMS and MoS_(2)/PMS *** results demonstrate that the presence of MoS_(2)under a water vortex can trigger a piezoelectric potential and generate abundant free electrons to activate PMS to generate various active species for degradation of organic contaminants.

关键词： Water vortex-driven Peroxymonosulfate utilization Piezoelectric activation Organic contaminants Few-odd-layered MoS2

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Enhanced persulfate activation process by magnetically separable catalysts for water purification:A review

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Chinese Journal of Structural Chemistry 2023年第6期42卷 55-67页

作者： Chuan Pu Gang Lu Hang Qi Abdulgalim B.Isaev mingshan zhu School of Environment Jinan UniversityGuangzhou510632China School of Environment and Energy Engineering Anhui Jianzhu University230601China Department of Inorganic Chemistry and Chemical Ecology Dagestan State UniversityM.Gadjieva 43a367001MakhachkalaRussian Federation

In recent years,persulfate(PS)-based advanced oxidation processes(AOPs)have become a hot research topic for degrading environmental pollutants due to their excellent oxidation capacity,selectivity,and ***-AOPs can generate sulfate radicals(SO^(·-)_(4))with strong oxidation ability,but single PS produces limited or no ***,activation of PS by energy input or catalyst dosing is used to improve its oxidation ***,the addition of disposable catalyst not only causes a waste of resources,but also may lead to secondary ***,magnetically separable catalysts for activating PS have received widespread attention due to their *** there are few literature reviews on the activation of PS by carbon-or iron-based magnetic materials,the mechanism analysis of the activation of PS by magnetic materials to degrade pollut-ants is not deep enough,and the discussion of material types is not comprehensive and ***,the discussion of magnetic materials in terms of recycling properties is ***,this review firstly sum-marizes and analyzes the mechanism of magnetically separable catalysts activating PS to degrade ***,the research progress of zero-valent iron(ZVI,Fe^(0))-based,iron oxide-based,bimetallic oxide-based,and other magnetically separable catalyst is introduced,and the tailoring engineering approaches and reusability of magnetically separable catalysts are ***,some possible material optimization suggestions are proposed in this *** conclusion,this review is expected to provide useful insights for improving the per-formance and reusability of magnetically separable materials activated PS in the future.

关键词： Magnetically separable catalysts AOPs Sulfate radicals Mechanism Reusability

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