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Science Bulletin 2025年第2期70卷 232-240页

作者： Wei Xia Zhijie Zhou Liangzheng Sheng Lihang Chen Fang Zheng Zhiguo Zhang Qiwei Yang Qilong Ren Zongbi Bao key laboratory of biomass chemical engineering of ministry of education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

The sequestration of trace hexafluoropropylene(C_(3)F_(6))is a critical yet formidable task in the production of high-purity perfluoropropane(C_(3)F_(8)),an important perfluorinated electronic specialty gas(F-gas)in the advanced electronics *** adsorbents struggle with uneven,low-pressure uptake and compromises in *** work utilizes aperture size-electrostatic potential matching within a robust metal–organic framework(Al-PMA)to facilitate selective,reversible binding of C_(3)F_(6)while excluding larger C_(3)F_(8)*** presence of bridging hydroxyl groups(μ_(2)-OH)in Al-PMA creates positive electrostatic potential traps that securely anchor C_(3)F_(6)through strong hydrogen bonding,evidenced by insitu infrared and^(19)F magic angle spinning nuclear magnetic resonance *** experiments demonstrate the efficient removal of trace C_(3)F_(6)from C_(3)F_(8)under ambient conditions,achieving C_(3)F_(8)purity exceeding 99.999%.The scalability of Al-PMA synthesis,remarkable stability,and exceptional performance highlight its potential as a promising adsorbent for industrial C_(3)F_(6)/C_(3)F_(8)separations.?2024 Science China *** by Elsevier *** Science China *** rights are reserved,including those for text and data mining,AI training,and similar technologies.

关键词： Deep purification Electronic specialty gas(ESGs) Metal-organic frameworks(MOFs) Positive potential traps(ppts)

Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang key laboratory of Green chemical engineering Process of ministry of education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina key laboratory of Pesticide&chemical Biology of ministry of education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina College of Materials Science and engineering Fuzhou UniversityFuzhou 350108FujianChina

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction(OER).Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER ***,most of them undergo incomplete reconstruction with limited thickness of reconstruction layer,leading to low component utilization and arduous exploration of real catalytic ***,we identify the dynamic behaviors in complete reconstruction of Co-based complexes during *** hollow phytic acid(PA)cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability,in favor of the fast and complete reconstruction.A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co(Fe)(OH)xand subsequent potential-driven oxidation to Co(Fe)*** obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm^(-2)and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER *** work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

Split crRNA-motivated amplification-free RNA testing with CRISPR-Cas12a

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Science China Chemistry 2025年第2期68卷 789-801页

作者： Jiayu Zeng Pengfei Liu Jinlian Du Sheng Li Erhu Xiong Ronghua Yang key laboratory of chemical Biology&Traditional Chinese Medicine Research Ministry of EducationCollege of Chemistry and Chemical EngineeringHunan Normal UniversityChangsha 410081China

The CRISPR RNA(crRNA)consists of a conserved repeat RNA(rRNA)and an alterable spacer RNA(sRNA),which can guide the Cas12a effector to recognize and target DNA molecules of interest in both full-length and split *** herein demonstrated the split crRNA can be repurposed for RNA detection through serving the sRNA as an RNA *** by this phenomenon,we developed a Cas12a-based direct RNA detection method,known as split crRNA-motivated amplification-free RNA testing(SMART).We adopted SMART to detect both short-stranded and long-stranded RNA target using two Cas12a orthologs(LbCas12a and FnCas12a),and it showed more prominent ability in detecting short-stranded RNA than long-stranded *** potential mechanism revealed that RNA overhangs impede the RNA strand and dsDNA activator from accessing the catalytic site in the RuvC domain of the Cas12a effector,compromising the stability of the quaternary complex,and thus reducing the efficiency of ***,by simply introducing a short DNA activator,SMART could detect attomolar miRNA targets and femtomolar long-stranded RNA target without the need for additional preamplification or reverse transcription *** addition,SMART showed wonderful discrimination ability toward single-nucleotide ***,the collaboration of SMART with the CRISPR–Cas13a system enabled simultaneous detection of multiplex ***,SMART is a simple,yet potent tool that can be flexibly applied to various short-stranded RNA detection,and holds great potential to be extended to other Cas12 orthologs.

关键词： RNA detection split crRNA CRISPR-Cas12a amplification-free miRNA

Optimizing the ORR performance of PtMnM ternary intermetallics by tuning the surface strain

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Science China Chemistry 2025年第2期68卷 536-542页

作者： Min Song Guanyu Luo Qian Zhang Hanyu Hu Deli Wang key laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074China

Identifying the descriptors that control catalytic performance is key to design catalysts with high activity and *** indirect descriptors related to catalytic activity,modulating the Pt–Pt interatomic distance and d-band center can effectively enhance the ORR *** is well recognized that the Pt–Pt interatomic distance is strongly correlated with the surface ***,PtMnM/C ternary intermetallics are constructed through partially replacing Mn in PtMn/C binary intermetallics with the other transition metal(M=Fe,Co,Ni,and Cu).The 3d-transition metal doping induces surface strain,and the ORR performance of PtMnM/C exhibits volcano relationship relative to both the Pt–Pt interatomic distance and d-band *** PtMnCo/C with optimum strain exhibits the highest mass activity(1.06 A mgPt^(−1))at 0.9 V,which is 2.6 and 4.6 times higher than that of PtMn/C and commercial Pt/C catalysts,*** addition,PtMnCo/C shows good durability with only 10 mV half-wave potential decay after 50,000 potential cycles.

关键词： oxygen reduction reaction electrocatalysts ternary intermetallics surface strain electronic structure

Metal nanoparticles decorated CoFe-(oxy)hydroxysulfides nanosheets fabricated by a general strategy for electrocatalytic water splitting

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Journal of Energy Chemistry 2025年第1期100卷 26-38页

作者： Xiaodong Yang Haochen Shen Xiaoming Xiao Zhichao Li Qi Zhou Wei Yang Bin Jiang Yongli Sun Luhong Zhang Zhenhua Yan School of chemical engineering and Technology Tianjin UniversityTianjin 300072China key laboratory of Advanced Energy Materials Chemistry(ministry of education) Nankai UniversityTianjin 300071China

This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization *** developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,*** both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 ***-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water ***,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER *** study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.

关键词： LDH Spontaneous reaction Metal nanoparticles Water splitting

Interfacial B-O bonding modulated S-scheme B-doped N-deficient C_(3)N_(4)/O-doped-C_(3)N_(5) for efficient photocatalytic overall water splitting

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Chinese chemical Letters 2025年第1期36卷 355-361页

作者： Entian Cui Yulian Lu Zhaoxia Li Zhilei Chen Chengyan Ge Jizhou Jiang key laboratory for Advanced Technology in Environmental Protection of Jiangsu Province Yancheng Institute of TechnologyYancheng 224051China School of Environmental Ecology and Biological engineering Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan 430205China

Photocatalytic overall pure water splitting is a promising method for generating green hydrogen energy under mild ***,this process is often hindered by sluggish electron-hole separation and *** address this,a step-scheme(S-scheme)B-doped N-deficient C_(3)N_(4)/O-doped C_(3)N_(5)(BN-C_(3)N_(4)/O-C_(3)N_(5))heterojunction with interfacial B-O bonds has been *** Pt and Co(OH)_(2) as co-catalysts,BN-C_(3)N_(4)/O-C_(3)N_(5) S-scheme heterojunction demonstrates significantly enhanced photocatalytic activity for overall pure water splitting under visible light,achieving H_(2) and O_(2) evolution rates of 40.12 and 19.62μmol/h,*** characterizations and experiments revealed the performance-enhancing effects of the enhanced built-in electric field and the interfacial B-O ***,the strengthened built-in electric field provides sufficient force for rapid interfacial electron ***,by reducing the transport energy barrier and transfer distance,the interfacial B-O bonds facilitate rapid recombination of electrons and holes with relatively low redox potential via the S-scheme charge-transfer route,leaving the high-potential electrons and holes available for H^(+)reduction and OH^(-)oxidation ***,the photocatalytic efficiency of BN-C_(3)N_(4)/O-C_(3)N_(5) S-scheme heterojunction was significantly improved,making it a promising approach for green hydrogen production through overall pure water splitting.

关键词： Interfacial B-O bonds BN-C_(3)N_(4) O-C_(3)N_(5) S-scheme heterojunction Water splitting

Pyrimidine derivative as eco-friendly corrosion inhibitor for nickel−aluminum bronze in seawater

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Transactions of Nonferrous Metals Society of China 2025年第1期35卷 207-224页

作者： Jin-yu PI Qi WANG Chao-yang FU key laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

A pyrimidine derivative,6-phenyl-2-thiouracil(PT),was synthesized for developing a corrosion inhibitor(CI)applied in the protection of the nickel−aluminum bronze(NAB)in *** anti-corrosion effect of PT was evaluated by the mass loss experiment,electrochemical tests and surface *** results show that PT exhibits excellent inhibition performance and the maximum inhibition efficiency of PT reaches 99.6%.The interaction mechanism was investigated through X-ray photoelectron spectroscopy(XPS)and molecule dynamics simulation based on the density functional theory(DFT).The S-Cu,Al-N and Cu-N bonds are formed by the chemical interactions,leading to the adsorption of PT on the NAB *** diffusion of corrosive species is hindered considerably by the protective PT film with composition of(PT-Cu)_(ads)and(PT-Al)_(ads)on the PT/NAB *** degree of suppression is increased with the addition of more PT molecules.

关键词： nickel−aluminum bronze corrosion inhibitor diffusion coefficient adsorption seawater

Investigation of spatiotemporal distribution and formation mechanisms of ozone pollution in eastern Chinese cities applying convolutional neural network

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Journal of Environmental Sciences 2025年第2期148卷 126-138页

作者： Qiaoli Wang Dongping Sheng Chengzhi Wu Xiaojie Ou Shengdong Yao Jingkai Zhao Feili Li Wei Li Jianmeng Chen 无 College of Environment Zhejiang University of TechnologyHangzhou 310032China key laboratory of biomass chemical engineering of the ministry of education Institute of Industrial Ecology and EnvironmentCollege of Chemical and Biological EngineeringZhejiang University(Zijingang Campus)Hangzhou 310027China Trinity Consultants Inc.(China office)Hangzhou 310012China Zhejiang University of Science&Technology Hangzhou 310023China

Severe ground-level ozone(O_(3))pollution over major Chinese cities has become one of the most challenging problems,which have deleterious effects on human health and the sustainability of *** study explored the spatiotemporal distribution characteristics of ground-level O_(3) and its precursors based on conventional pollutant and meteorological monitoring data in Zhejiang Province from 2016 to ***,a high-performance convolutional neural network(CNN)model was established by expanding the moment and the concentration variations to general ***,the response mechanism of O_(3) to the variation with crucial influencing factors is explored by controlling variables and interpolating target *** results indicated that the annual average MDA8-90th concentrations in Zhejiang Province are higher in the northern and lower in the *** the wind direction(WD)ranges from east to southwest and the wind speed(WS)ranges between 2 and 3 m/sec,higher O_(3) concentration prone to *** different temperatures(T),the O_(3) concentration showed a trend of first increasing and subsequently decreasing with increasing NO_(2) concentration,peaks at the NO_(2) concentration around 0.02mg/m^(3).The sensitivity of NO_(2) to O_(3) formation is not easily affected by temperature,barometric pressure and dew point ***,there is a minimum IRNO_(2) at each temperature when the NO_(2) concentration is 0.03 mg/m^(3),and this minimum IRNO_(2) decreases with increasing *** study explores the response mechanism of O_(3) with the change of driving variables,which can provide a scientific foundation and methodological support for the targeted management of O_(3) pollution.

关键词： Ozone Spatiotemporal distribution Convolutional neural network Ozone formation rules Incremental reactivity

Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO_(2)reduction to C2þchemicals

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Green Energy & Environment 2025年第2期10卷 422-432页

作者： Wenrui Wan Fanhua Meng Si Chen Jianhua Wang Chunyan Liu Yan Wei Chenpu He Li Fan Qiaolan Zhang Weichun Ye Huanwang Jing State key laboratory of Applied Organic Chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000GansuChina key laboratory of Green chemical Media and Reactions(ministry of education) School of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang453007HenanChina School of chemical engineering Lanzhou University of Arts and SciencesLanzhou730010China

Converting CO_(2)and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy *** inspiration from the structures of natural leaves,we designed and synthesized a novel copper-coordinated covalent triazine framework(CuCTF)supported by silicon nanowire arrays on wafer *** marks the first-ever application of such a hybrid material in the photoelectrocatalytic reduction of CO_(2)under mild *** Si@CuCTF6 heterojunction has exhibited exceptional selectivity of 95.6%towards multicarbon products(C^(2+))and apparent quantum efficiency(AQE)of 0.89%for carbon-based *** active sites of the catalysts are derived from the nitrogen atoms of unique triazine ring structure in the ordered porous framework and the abundant Cu-N coordination sites with bipyridine ***,through DFT calculations and operando FTIR spectra analysis,we proposed a comprehensive mechanism for the photoelectrocatalytic CO_(2)reduction,confirming the existence of key intermediate species such as*CO_(2)-,*=C=O,*CHO and*CO-CHO *** work not only provides a new way to mimic photosynthesis of plant leaves but also gives a new opportunity to enter this research field in the future.

关键词： Silicon Photoelectrocatalysis CO_(2)reduction Covalent triazine framework Sustainable chemistry

Classification and progress of extraction technologies for nonferrous metal resources

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Science China Chemistry 2025年第2期68卷 458-474页

作者： Fangqin Cheng Na Zhou Nazeer Muhammad Nouman Li Cui Caixia Yin Institute of Resources and Environmental engineering State Environmental Protection Key Laboratory of Efficient Utilization of Coal Waste ResourcesShanxi UniversityTaiyuan 030006China key laboratory of chemical Biology and Molecular engineering of ministry of education Institute of Molecular ScienceShanxi UniversityTaiyuan 030006China

In recent years,the demand for strategic metal resources,essential for scientific and technological progress and industrial development,has *** a stable supply of these metals is critical to national security and the well-being of the *** global industrialization accelerates,the daily demand for nonferrous metals continues to ***,extracting and recovering strategic metals from low-grade raw materials,such as solid waste,has become crucial for maintaining their supply and economic ***,the extraction process is fraught with challenges,including mineral phase stability and complex *** review focuses on key strategic metals such as lithium,aluminum,gallium,and *** introduces and examines various methods for extracting nonferrous metals from different raw materials,including traditional mining technologies applied to low-grade solid *** also outlines future development opportunities and challenges in this field.

关键词： nonferrous metal extraction classification and progress