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Potential industrial applications of photo/electrocatalysis: Recent progress and future challenges

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Green Energy & Environment 2024年第5期9卷 859-876页

作者： Jinhao Li Jing Ren Shaoquan Li Guangchao Li Molly Meng-Jung Li Rengui Li Young Soo Kang Xiaoxin Zou Yong Luo Bin Liu Yufei Zhao State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China Quzhou institute for Innovation in Resource Chemical Engineering Quzhou324000China State Key Laboratory of Organic-inorganic Composites Beijing University of Chemical TechnologyBeijing100029China Department of Applied Physics The Hong Kong Polytechnic UniversityHong Kong999077China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian National Laboratory for Clean EnergyZhongshan Road 457Dalian116023China Environmental and Climate Technology Track of Korea institute of Energy Korea Institute of Energy TechnologyNaju-siJeollanam do58217Republic of Korea State Key Laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun130012China

Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental crisis.For this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis technology for the advantage in the sustainable production of high-value-added products,and the high efﬁciency in pollutants remediation.Although there is plenty of outstanding research has been put forward continuously,most of them focuses on catalysis performance and reaction mechanisms in laboratory conditions.Realizing industrial application of photo/electrocatalytic processes is still a challenge that needs to be overcome by social demand.In this regard,this review comprehensively summarized several explorations in theﬁeld of photo/electrocatalytic reduction towards potential industrial applications in recent years.Special attention is paid to the successful attempts and the current status of photo/electrocatalytic water splitting,carbon dioxide conversion,resource utilization from waste,etc.,by using advanced reactors.The key problems and challenges of photo/electrocatalysis in future industrial practice are also discussed,and the possible development directions are also pointed out from the industry view.

关键词： Photocatalysis Electrocatalysis Industrial applications H2 economy

A Golden Touch in the Design of Multifunctional Porphyrin Metallacages:Host-Guest chemistry for Drug-Target Interactions

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CCS chemistry 2024年第7期6卷 1662-1671页

作者： Tamara Rodríguez-Prieto Darren Wragg Nicole Heiduk Mihyun Park Nicole Strittmatter Roland A.Fischer Angela Casini Guillermo Moreno-Alcántar Chair of Medicinal and Bioinorganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Professorship for Analytical chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Chair of inorganic and MetalOrganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Munich Data Science institute(MDSI) Technical University of Munich85748 Garching b.München

The use of three-dimensional self-assembled metallacages(MCgs)as multimodal drug platforms holds great promise.However,the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still limited.In this context,this work reports on the integration of a gold(III)porphyrin scaffold into a prismatic MCg structure and explores its application for multimodal therapy of cancer in vitro,namely enabling both photodynamic therapy and chemotherapy.Combining experimental approaches with a state-of-the-art metadynamics theoretical study,we discovered that the gold cage shows unprecedented host-guest interaction-driven selective stabilization of guanine-quadruplex(G4)structures-validated anticancer drug targets-disclosing a new mechanism to pursue in the design of supramolecular drugs.

关键词： gold metallacages porphyrins G4stabili-zation host-guestchemistry anticanceragents

Advancements in synthetic and electrocatalytic exploitation of guest-host intercalated 2D materials

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Progress in Natural Science:Materials International 2024年第3期34卷 454-469页

作者： Qian Yang Kun Wang Meiling Zhang Feihong Du Jiayang Li Chen Zheng Jinyang Li School of chemistry Southwest Jiaotong University Yibin institute of Southwest Jiaotong University

The emergence and development of layered materials have shown great promise for many applications, especially in recent years, the effective modulation of the physicochemical properties of layered materials by intercalation chemistry has led to great potential in material design. In this paper, we review the reaction mechanisms of different guest species(metal atoms/ions, organic molecules/ions, inorganic molecules and inorganic ions)intercalated into the host layered materials as well as the recent progress. It is also reviewed that layered intercalated materials with controllable structure and tunable physicochemical properties can be prepared through the occurrence of interactions between different subjects and guests. The specific applications of intercalation chemistry in the field of electrocatalysis, such as the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction and other electrocatalytic reactions, are then discussed, with emphasis on the mechanism of the improved catalytic activity and stability of the layered materials after guest intercalation.

关键词： Electrocatalysis Guest species Intercalation chemistry Layered materials

Phosphine-Catalyzed [4+3] Annulation Reaction of Indole Derivatives with MBH Carbonates:A Facile Access to Indole-1,2-fused 1,4-Diazepinones and Azepines

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Chinese Journal of chemistry 2024年第3期42卷 271-275页

作者： Yannan Zhu Haoran Jiang Yi-Ning Wang Faculty of chemistry and Chemical Engineering Yancheng Institute of TechnologyYanchengJiangsu224051 China

A phosphine-catalyzed [4+3] annulation between dinucleophilic indole derivatives and Morita−Baylis−Hillman (MBH) carbonates was discovered by using the N1 and N4′/C4′ nucleophilicities of the indole precursors,in which indoles act as four atom synthons. This protocol provides an efficient and facile access to indole-1,2-fused 1,4-diazepinones and azepines in good to high yields in one step,which illustrates potential synthetic utilities in drug discovery.

关键词： Phosphine catalysis [4+3]Annulation Indole derivatives Nitrogen heterocycles Organocatalysis

Pd-catalyzed intermolecular Si–O formation via Si–C activation

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Science China chemistry 2024年第8期67卷 2661-2669页

作者： Shuang Liu Yu-Shu Chen Yichen Wu Peng Wang State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences School of chemistry and Materials Science Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences College of Material chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education Hangzhou Normal University

The development of efficient Si–O bond formation reaction with 100% atom-economy, excellent functional group tolerance, and broad scope under mild conditions is highly desired due to the prevalence of silanol, silyl ether, and their derivatives in synthetic chemistry and materials science. Here, we have realized the Pd-catalyzed Si–O formation reaction via a Si–C activation approach with 100% atom-economy by employing silacyclobutanes(SCBs) and various hydroxy-containing substrates, including water,alcohols, phenols, and silanols. This protocol features a broad substrate scope, remarkable functional compatibility and mild conditions, providing a series of silanols, silyl ethers in high efficiency. Notably, this protocol could also be used for selective protection of hydroxy functionalities, and for the access of a class of novel polymers containing Si–O main chain. Preliminary mechanistic studies unveiled that this reaction underwent a Pd-catalyzed concerted ring-opening mechanism.

关键词： palladium silacyclobutane silanol silyl ether Si–C activation Si–O formation

Mass transfer in heap leaching of weathered crust elution deposited rare earth ore with Al_(2)(SO_(4))_(3) solution

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Journal of Rare Earths 2024年第6期42卷 1175-1181,I0007页

作者： Jingqun Yin Dedong Zeng Jun Tian Yaqing Weng institute of Applied chemistry Jiangxi Academy of SciencesNanchang330096China School of chemistry and Chemical Engineering Nanchang UniversityNanchang330031China

In order to increase efficiency and avoid NH^(4+)-N pollution in the leaching process of weathered crust elution-deposited rare earth ores,the mass transfer in heap leaching with Al_(2)(SO_(4))_(3) solution was simulated with column elution and experimentally optimized.The results indicate that the leaching yield is also up to 99%for leaching with aluminum sulfate instead of ammonium sulfate.The optimal flow rate is 60 mL/h,the height equivalent to a theoretical plate(HETP)is 1.29 mm correspondingly.The peak value position of RE^(3+)is 60 mL/h,Fe^(3+)is 100 mL/h,however,Al^(3+)is 150 mL/h,and the heap leaching process has kinetic separation effect.

关键词： Raree arths Mass transfer Process optimization Heapleaching Weathered crust elution-deposited rare earth ore

Effects of surface chlorine atoms on charge distribution and reaction barriers for photocatalytic CO_(2)reduction

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Nano Materials Science 2024年第2期6卷 235-243页

作者： Wendong Zhang Wenjun Ma Yuerui Ma Peng Chen Qingqing Ye Yi Wang Zhongwei Jiang Yingqing Ou Fan Dong Chongqing Key Laboratory of Green Synthesis and Application&Chongqing Key Laboratory of inorganic Functional Materials College of ChemistryChongqing Normal UniversityChongqing401331China Suzhou Industrial Technology Research institute of Zhejiang University Jiangsu215000China Department of chemistry Faculty of ScienceNational University of SingaporeSingapore117543Singapore Yangtze Delta Region institute(Huzhou)&institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaHuzhou313001China

Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst.

关键词： Surface chlorine atoms Charge distribution Reaction barriers Photocatalytic CO_(2)reduction Bi_(2)WO_(6)

Stabilization and detection of labile reaction intermediates in supramolecular containers

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Chinese Chemical Letters 2024年第6期35卷 47-52页

作者： Rui Wang Yang Liang Julius Rebek Jr. Yang Yu Center for Supramolecular chemistry&Catalysis and Department of chemistry College of ScienceShanghai UniversityShanghai 200444China Skaggs institute for Chemical Biology and Department of chemistry The Scripps Research InstituteLa JollaCA 92037United States

Detection and observation of reactive intermediates is an essential step in investigation of reaction pathways.However,most reactive intermediates are unstable and present at low concentrations;their short lifetimes make them difficult to detect and characterize.Supramolecular containers offer opportunities for the stabilization and characterization of those labile species,through isolation from the media and protection inside the cavity of the host.In this review,we summarize the examples of labile reaction intermediates that are stabilized and characterized with the help of supramolecular containers.The container compounds include carcerands,deep cavitands and amide naphthotubes.We focus on unstable guest species-cyclobutadiene,benzocyclopropenone,o-benzyne,1,2,4,6-cycloheptatetraene,anti-Bredt's olefin,fluorophenoxycarbene,O-acylisoamide,and hemiaminalthat act as intermediates in certain organic reactions.

关键词： Supramolecular containers Reaction intermediates Labile species stabilization Short-lived species detection Supramolecular chemistry

Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

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National Science Review 2024年第2期11卷 155-167页

作者： Peng He Meng-Yang Hu Jin-Hong Li Tian-Zhang Qiao Yi-Lin Lu Shou-Fei Zhu Frontiers Science Center for New Organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation