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Efficient and selective h_(2)O_(2)production through uranyl-assisted photocatalytic oxygen reduction reaction process in a uranium-organic framework

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Science China Chemistry 2024年第7期67卷 2274-2281页

作者： Jianxin Song chao Liang Baoyu Li Xuemin Wang Min Lei Lisha Jiang Zhenyu Li Yugang Zhang Jian Xie Zuju Ma Xing Dai Yanlong Wang Shuao Wang Wei Liu School of Environmental and Materials Engineering Yantai UniversityYantai 264005China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China School of Life and Environmental Sciences Shaoxing UniversityShaoxing 312000China School of Nuclear Science and Technology Xi’an Jiaotong UniversityXi’an 710049China

harnessing solar energy by photocatalytically converting oxygen and water into high-value-added h_(2)O_(2)is a promising way of alleviating both environmental and energy *** is worth noting that suppressing detrimental side reactions,such as the generation of·O_(2)^(-),is a critical approach to enhancing h_(2)O_(2)***,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic h_(2)O_(2)*** material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge *** from the strong hydrogen abstraction effect of the U≡O·and the direct one-step oxygen reduction pathway,YTU-W-1 exhibits enhanced photocatalytic performance for h_(2)O_(2)production with yield efficiency of 221μmol h^(-1)g^(-1).Furthermore,YTU-W-1 displays a high h_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)*** were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for h_(2)O_(2)*** research introduces an innovative approach to photo-driven h_(2)O_(2)production,underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photogenerated charge carriers.

关键词： uranyl metal-organic frameworks oxygen reduction reaction photocatalytic h_(2)O_(2)synthesis

Boosting Electrochemical Urea Synthesis via Constructing Ordered Pd–Zn Active Pair

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Nano-Micro Letters 2024年第11期16卷 529-540页

作者： Weiliang Zhou chao Feng Xuan Li Xingxing Jiang Lingyan Jing Shuai Qi Qihua huo Miaoyuan Lv Xinbao Chen Tianchi huang Jingwen Zhao Na Meng hengpan Yang Qi hu Chuanxin he College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongPeople’s Republic of China School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832003XinjiangPeople’s Republic of China

Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained ***,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea *** is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn *** importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical ***,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn *** work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.

关键词： Electrochemical C-N coupling Urea electrosynthesis Intermetallic compounds Geometric structures Active pairs

“半城半牧”:牧区两栖式城镇化发展特点与成因剖析——基于青海省h县的调查

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青海社会科学 2024年第2期 61-67页

作者：刘超四川大学公共管理学院

实现以人为核心的新型城镇化是中国式现代化的必由之路和重要标志,也是推动民族地区经济社会文化发展的驱动力。青海省h县地方政府将移民工程与城镇化发展战略相结合,将牧区人口向小城镇集中,形成了“两栖式”新型城镇化,表现为城镇与... 详细信息

实现以人为核心的新型城镇化是中国式现代化的必由之路和重要标志,也是推动民族地区经济社会文化发展的驱动力。青海省h县地方政府将移民工程与城镇化发展战略相结合,将牧区人口向小城镇集中,形成了“两栖式”新型城镇化,表现为城镇与牧区互动频繁化,牧民生计模式多元化与生活方式城市化,其形成是畜牧业生产经营模式的发展性、县域公共服务的集中性与县城生活的丰富性等多元因素综合作用的结果。相较而言,牧民作为“能动的主体”嵌入中国式城乡二元结构,并且“半城半牧”的城镇化形态形成了草原牧区与城市社区的有机互动,有利于实现生态治理、民生保障与经济发展的系统目标。

关键词：牧区城镇化两栖式半城半牧生态治理

Two-Dimensional Conductive Metal-Organic Framework Reinforced Spinterface in Organic Spin Valves

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CCS Chemistry 2024年第1期6卷 208-217页

作者： Xiaoyu Song chao Jin hongliang Chen Shuaishuai Ding Zhongyi Liu Yang Li Xiaoli Yan Wenbo Mi Long Chen Wenping hu Department of Chemistry Tianjin Key Laboratory of Molecular Optoelectronic ScienceTianjin UniversityTianjin 300072 School of Chemistry and Chemical Engineering Yantai UniverisityYantaiShandong 264005 Tianjin Key Laboratory of Low Dimensional Materials Physics and Processing Technology School of ScienceTianjin UniversityTianjin 300072 State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchunJilin 130012

Interface engineering in device fabrication is a significant but complicated *** great successes have been achieved by conventional physical in situ or ex situ methods,it still suffers from complicated *** this work,we present a facile method for fabricating phthalocyanine(Pc)-based two-dimensional conductive metal–organic framework(MOF)*** on PcM-Cu(M=Ni,Cu,h_(2))MOF films,spin valves with a vertical configuration of La_(0.67)Sr_(0.33)MnO_(3)/PcM-Cu MOFs/Co were constructed successfully,and exhibited notably high negative magnetoresistance(MR)up to -22% at 50 *** penetrated Co atoms coordinated with the dehydrogenated hydroxy groups in the MOFs resulting in an antiferromagnetic layer of the PcM-Cu-Co hybrid ***,a significant exchange bias effect was demonstrated at the PcM-Cu MOF/Co interface,beneficial for the MR ***,our present study provides new insights into developing high-performance organic spin valves via de novo molecular design.

关键词： two-dimensional conductive metal-organic framework two-dimensional polymer phthalocyanine spintronics organic spin valve

Efficient solar-driven CO_(2)-to-fuel conversion via Ni/MgAlO_(x)@SiO_(2)nanocomposites at low temperature

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Fundamental Research 2024年第1期4卷 131-139页

作者： Xianglei Liu Yueyue Ling Chen Sun hang Shi hangbin Zheng chao Song Ke Gao Chunzhuo Dang Nan Sun Yimin Xuan Yulong Ding School of Energy and Power Engineering Nanjing University of Aeronautics and AstronauticsNanjing 210016China Birmingham Centre for Energy Storage School of Chemical EngineeringUniversity of BirminghamBirmingham B152TTUnited Kingdom

Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas Ch_(4)is promising to concurrently tackle energy shortage and global warming ***,current techniques still suffer from drawbacks of low efficiency,poor stability,and low ***,a novel nanocomposite composed of interconnected Ni/MgAlOx nanoflakes grown on SiO_(2)particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO_(2)-to-fuel *** ultrahigh light-to-fuel efficiency up to 35.7%,high production rates of h_(2)(136.6 mmol min^(-1)g^(-1))and CO(148.2 mmol min^(-1)g^(-1)),excellent selectivity(h_(2)/CO ratio of 0.92),and good stability are reported *** outstanding performances are attributed to strong metal-support interactions,improved CO_(2)absorption and activation,and decreased apparent activation energy under direct light ***_(x)@SiO_(2)support helps to lower the activation energy of Ch^(*) oxidation to ChO^(*) and improve the dissociation of Ch_(4)to Ch_(3)^(*) as confirmed by DFT ***,the lattice oxygen of MgAlO_(x) participates in the reaction and contributes to the removal of carbon *** work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency,high selectivity,and benign sustainability.

关键词： Solar fuel CO_(2)reduction Dry reforming of methane Photothermocatalysis Stability

Bifunctional electrolyte addition for longer life and higher capacity of aqueous zinc-ion hybrid supercapacitors

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Rare Metals 2024年第10期43卷 5060-5069页

作者： Fan Zhang Si-Qi Li Li-Nan Xia chao Yang Lei Li Kai-Ming Wang Chen-Liang Xu Yuan-Yuan Feng Bin Zhao Fei Shen Xiao-Gang han Ling-Yun Zhu School of Electric Power Civil Engineering and ArchitectureShanxi University State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical EngineeringXi’an Jiaotong University Department of Science Materials and Engineering National University of Singapore School of Materials Science and Engineering Anhui University

Owing to uncontrolled and uneven electrodeposition and side reactions,Zn metal anodes inevitably suffer from issues such as dendrite growth,hydrogen evolution reactions,and surface *** paper proposes an efficient strategy to address these critical issues for realizing long-life and high-capacity aqueous zinc-ion hybrid supercapacitors （ZhSCs） by incorporating low-concentration (0.05 mol·L-1) redox RbI electrolyte ***,rubidium cations have the ability to influence the negative Zn electrode surface via an electrostatic shielding mechanism,effectively protecting the electrode and minimizing undesired side *** an aqueous solution,iodide anions actively solvate Zn2+ions by stabilizing and modulating the solvation shell surrounding Zn2+.Moreover,the presence of iodide ions promotes the uniform deposition of Zn2+species by selective adsorption onto the electrode *** synergistic effect of the electrostatic shielding and halogen ions enables the realization of aqueous symmetric Zn||Zn cells with a substantial cycle life of more than 2000 h Additionally,when applied to commercial activated carbon（AC）,the proposed strategy facilitates the development of aqueous ZhSCs,exhibiting high specific capacitances(148.8 F·g-1at 4 A·g-1) and ultra-long cycling stability.

关键词： Aqueous zinc-ion hybrid supercapacitor Rubidium iodide Synergistic effects of anions and cations Zn dendrite Zn metal anode

Expanding the targeting scope of CRISPR/Cas9-mediated genome editing by Cas9 variants in Brassica

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aBIOTECh 2024年第2期5卷 202-208页

作者： Wenjing Li Xuan Li Chunyang Wang Guanzhong huo Xinru Zhang Jintai Yu Xiaoxiao Yu Jing Li chao Zhang Jianjun Zhao Yan Li Jun Li State Key Laboratory of North China Crop Improvement and Regulation College of Life SciencesHebei Agricultural UniversityBaoding 071001China hebei Key Laboratory of Plant Physiology and Molecular Pathology Hebei Agricultural UniversityBaoding 071001China Key Laboratory of Vegetable Germplasm Innovation and Utilization of hebei Collaborative Innovation Center of Vegetable Industry in HebeiCollege of HorticultureHebei Agricultural UniversityBaoding 071001China College of Modern Science and Technology Hebei Agricultural UniversityBaoding 071001China

CRISPR/Cas9,presently the most widely used genome editing technology,has provided great potential for functional studies and plant ***,the strict requirement for a protospacer adjacent motif(PAM)has hindered the application of the CRISPR/Cas9 system because the number of targetable genomic sites is ***,the engineered variants Cas9-NG,SpG,and SpRY,which recognize non-canonical PAMs,have been successfully tested in plants(mainly in rice,a monocot).In this study,we evaluated the targeted mutagenesis capabilities of these Cas9 variants in two important Brassica vegetables,Chinese cabbage(Brassica rapa ***)and cabbage(Brassica oleracea ***).Both Cas9-NG and SpG induced efficient mutagenesis at NGN PAMs,while SpG outperformed Cas9-NG at NGC and NGT *** achieved efficient editing at almost all PAMs(NRN>NYN),albeit with some self-targeting activity at transfer(T)-DNA *** SpRY-induced mutants were detected in cabbage plants in a PAM-less ***,an adenine base editor was developed using SpRY and TadA8e deaminase that induced A-to-G conversions within target sites using non-canonical ***,the toolboxes developed here induced successful genome editing in Chinese cabbage and *** work further expands the targeting scope of genome editing and paves the way for future basic research and genetic improvement in Brassica.

关键词： Brassica Cas9 variants CRISPR Genome editing Non-canonical PAM

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含挖填界面边坡三维稳定性上限分析

岩土工程学报 2024年第1期46卷 174-181页

作者：闫超王红雨宁夏大学土木与水利工程学院宁夏银川750021

针对工程实践中挖填交界面与边坡坡面走向线斜交的高边坡空间三维稳定分析问题,基于极限分析上限定理,构建拓展的三维牛角状破坏机构,通过引入机构参数挖填界面倾角α突出边坡特性,建立与之对应的功能平衡方程,采用序列二次规划优化算... 详细信息

针对工程实践中挖填交界面与边坡坡面走向线斜交的高边坡空间三维稳定分析问题,基于极限分析上限定理,构建拓展的三维牛角状破坏机构,通过引入机构参数挖填界面倾角α突出边坡特性,建立与之对应的功能平衡方程,采用序列二次规划优化算法求解强度折减后的边坡安全系数上限解。在此基础上,计算了宁夏黄土丘陵地区妙岭750kV变电站高边坡以及相关文献中极限状态下边坡稳定性系数γh/c工程案例,并将计算结果与有限元极限分析软件模拟值进行对比分析。结果表明:随着挖填界面倾角α的增大,边坡安全系数Fs上限解和模拟值均减小,两种方法的计算结果相对误差在5.9%以内,且拓展的破坏机构与数值模拟的剪切耗散变形模式基本一致;在极限状态下,拓展机构的上限解和数值模拟结果都十分接近于1.0,二者相对误差未超过8.3%。研究工作为此类高边坡空间稳定分析问题提供了一种简便实用的计算方法。

关键词：边坡稳定性上限分析挖填界面三维效应安全系数

Enhanced reversible hydrogen storage properties of wrinkled graphene microflowers confined LiBh_(4) system with high volumetric hydrogen storage capacity

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Materials Reports(Energy) 2024年第1期4卷 79-88页

作者： Zhenglong Li Kaicheng Xian hao Chen Mingxia Gao Shanqing Qu Meihong Wu Yaxiong Yang Wenping Sun chao Gao Yongfeng Liu Xin Zhang hongge Pan Institute of Science and Technology for New Energy Xi'an Technological UniversityXi'an710021PR China State Key Laboratory of Silicon and Advanced Semiconductor Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang ProvinceSchool of Materials Science and EngineeringZhejiang UniversityHangzhou310027PR China Department of Polymer Science and Engineering MOE Key Laboratory of Macromolecular Synthesis and FunctionalizationZhejiang UniversityHangzhou310027PR China

LiBh_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage ***,it suffers from high dehydrogenation temperature and poor reversibility for practical *** is effective in achieving low dehydrogenation temperature and favorable ***,graphene can serve as supporting materials for LiBh_(4)catalysts and also destabilize LiBh_(4)via interfacial ***,graphene has never been used alone as a frame material for nanoconfining LiBh_(4).In this study,graphene microflowers with large pore volumes were prepared and used as nanoconfinement framework material for LiBh_(4),and the nanoconfinement effect of graphene was *** loading 70 wt%of LiBh_(4) and mechanically compressed at 350 MPa,8.0 wt% of h2 can be released within 100 min at 320C,corresponding to the highest volumetric hydrogen storage density of 94.9 g h2 L^(-1)ever *** to the nanoconfinement of graphene,the rate-limiting step of dehydrogenation of nanoconfined LiBh_(4) was changed and its apparent activation energy of the dehydrogenation(107.3 kJ mol^(-1))was 42%lower than that of pure LiBh_(4).Moreover,the formation of the intermediate Li_(2)B_(12)h_(12) was effectively inhibited,and the stable nanoconfined structure enhanced the reversibility of LiBh_(4).This work widens the understanding of graphene's nanoconfinement effect and provides new insights for developing high-density hydrogen storage materials.

关键词： hydrogen storage LiBh_(4) Nanoconfinement Graphene high capacity