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Simulation-guided atomic Ni catalyst with oxygen-enriched coordination environment for H2O2 electrosynthesis coupled with 5-HMF oxidation 具有富氧配位环境的仿真引导原子镍催化剂用于 H2O2 电合成及 5-HMF 氧化
IF 9.4
Chem Catalysis Pub Date : 2024-08-26 DOI: 10.1016/j.checat.2024.101090
Jun Wang, Xiaomei Liu, Chengbo Ma, Huanyu Fu, Shuo Chen, Ning Li, Yang Li, Xiaobin Fan, Wenchao Peng
{"title":"Simulation-guided atomic Ni catalyst with oxygen-enriched coordination environment for H2O2 electrosynthesis coupled with 5-HMF oxidation","authors":"Jun Wang, Xiaomei Liu, Chengbo Ma, Huanyu Fu, Shuo Chen, Ning Li, Yang Li, Xiaobin Fan, Wenchao Peng","doi":"10.1016/j.checat.2024.101090","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101090","url":null,"abstract":"<p>The electrosynthesis of H<sub>2</sub>O<sub>2</sub> production via the two-electron oxygen reduction reaction (2e-ORR) has attracted increasing attention. In this work, a novel Ni-N-C single-atom catalyst (SAC) with Ni-N<sub>4</sub>O<sub>1</sub> coordination and a C-O-C synergistic structure is screened out. The corresponding SAC is then synthesized via chelation annealing. During the 2e-ORR test, the Ni-NOC exhibits an H<sub>2</sub>O<sub>2</sub> selectivity of 92.7% at 0.5 V vs. reversible hydrogen electrode (RHE), and the H<sub>2</sub>O<sub>2</sub> production rate can reach 252.91 mmol h<sup>−1</sup> g<sup>−1</sup> with a TOF of 0.187 s<sup>−1</sup>, which is among the best Ni-N-C catalysts. In addition, the cathodic 2e-ORR on this SAC is successfully coupled with the anodic oxidation of 5-HMF, and an overpotential of 0.32 V is achieved for 5-HMF oxidation at 50 mA, much smaller than the traditional oxygen evolution reaction (OER) process. Hence, this work provides a promising strategy for designing highly active 2e–ORR SACs as well as a novel coupling system of H<sub>2</sub>O<sub>2</sub> production and 5-HMF electrooxidation.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085257","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Photobiocatalysis: More than just an interesting lab curiosity? 光生物催化：不仅仅是有趣的实验室好奇心？
IF 9.4
Chem Catalysis Pub Date : 2024-08-23 DOI: 10.1016/j.checat.2024.101077
Yunjian Ma, Yutong Wang, Bin Wu, Jianle Zhou, Shunong Yang, Fangyu Zhang, Keyu Luo, Yonghua Wang, Frank Hollmann
{"title":"Photobiocatalysis: More than just an interesting lab curiosity?","authors":"Yunjian Ma, Yutong Wang, Bin Wu, Jianle Zhou, Shunong Yang, Fangyu Zhang, Keyu Luo, Yonghua Wang, Frank Hollmann","doi":"10.1016/j.checat.2024.101077","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101077","url":null,"abstract":"<p>Photobiocatalysis is currently in vogue. The number of reports combining the disciplines of biocatalysis and photocatalysis is rapidly increasing. While the synthetic possibilities enabled by photobiocatalysis are fascinating, the economic feasibility and environmental impact are largely neglected in the current literature. In this contribution, we present a range of key indicators for economic feasibility and environmental impact that may be useful for readers to assess their own work and thereby avoid unrealistic exaggerations. We also critically review the current state of the art in photobiocatalysis and question its synthetic practicability beyond the laboratory. With this contribution, we aim to provoke an open discussion.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142043307","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Understanding non-covalent interactions in Ni-catalyzed reactions: Mechanistic insights into stereoselective tetrasubstituted allene synthesis 了解镍催化反应中的非共价相互作用：立体选择性四取代烯合成的机理启示
IF 9.4
Chem Catalysis Pub Date : 2024-08-20 DOI: 10.1016/j.checat.2024.101082
Seoyeon Kim, Da Seul Lee, Naeem Iqbal, Jaehan Bae, Ho Seong Hwang, Doohyun Baek, Sukwon Hong, Eun Jin Cho
{"title":"Understanding non-covalent interactions in Ni-catalyzed reactions: Mechanistic insights into stereoselective tetrasubstituted allene synthesis","authors":"Seoyeon Kim, Da Seul Lee, Naeem Iqbal, Jaehan Bae, Ho Seong Hwang, Doohyun Baek, Sukwon Hong, Eun Jin Cho","doi":"10.1016/j.checat.2024.101082","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101082","url":null,"abstract":"<p>We report a nickel-catalyzed approach for the efficient synthesis of tetrasubstituted allenes from tertiary propargylic substrates, which remains a significant challenge due to competing substitution reactions and regioselectivity issues. Leveraging an optimized Ni-PˆN catalytic system, the notable non-covalent interactions (NCIs) overcome inherent stability issues and achieve regio- and stereoselectivity. Through a combination of experimental and computational analyses, we elucidate the stabilization mechanisms of the critical <em>β</em>-[Ni]-alkenyl intermediate from the reactions of arylated propargyl substrates. Our findings demonstrate that NCIs, in particular hydrogen bonding interactions between a unique free amino-type PˆN ligand and the substrate, are key to achieving precise control over the process. The efficiency of the process is greatly influenced by subtle differences in the ligand system through control of the bite angle and coordination length in the key nickel complex intermediates.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Controlling hydrogen transfer dynamics in adaptive semihydrogenation of alkynes: Unveiling and directing outer- vs. inner-sphere mechanisms 控制炔烃自适应半氢化过程中的氢转移动力学：揭示和引导外球与内球机制
IF 9.4
Chem Catalysis Pub Date : 2024-08-20 DOI: 10.1016/j.checat.2024.101078
Vishal Chugh, Jiajun Wu, Markus Leutzsch, Helena Randel, Thomas Weyhermüller, Alexander A. Auer, Christophe Farès, Christophe Werlé
{"title":"Controlling hydrogen transfer dynamics in adaptive semihydrogenation of alkynes: Unveiling and directing outer- vs. inner-sphere mechanisms","authors":"Vishal Chugh, Jiajun Wu, Markus Leutzsch, Helena Randel, Thomas Weyhermüller, Alexander A. Auer, Christophe Farès, Christophe Werlé","doi":"10.1016/j.checat.2024.101078","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101078","url":null,"abstract":"<p>This research presents an adaptive catalyst engineered to optimize hydrogen activation and transfer, demonstrated through its application in the semihydrogenation of alkynes. The catalyst is distinguished by a unique ligand pocket that precisely manipulates H₂ dynamics and substrate interactions. Its ability to adjust to solvent variations ensures the selective synthesis of <em>cis-</em> and <em>trans-</em>alkenes directly from alkynes without reliance on selectivity-altering additives. Our extensive mechanistic study sheds light on the critical influence of the solvent in guiding hydrogen transfer mechanisms, revealing an unconventional outer sphere hydrogenation process. The reversible nature of the catalyst and its robust performance over repeated cycles represent a significant advancement in controlled hydrogen catalysis. This progress highlights the feasibility of selectively producing both kinetic and thermodynamic products, setting a new standard for efficiency and versatility in catalytic processes.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The role of size and structure of catalytic active sites in polyolefin hydrogenolysis 催化活性位点的大小和结构在聚烯烃氢解中的作用
IF 9.4
Chem Catalysis Pub Date : 2024-08-20 DOI: 10.1016/j.checat.2024.101076
Jueun Kim, Simin Sun, Donghyeon Kim, Byung Gwan Park, Hojeong Lee, Wenyu Huang, Kwangjin An
{"title":"The role of size and structure of catalytic active sites in polyolefin hydrogenolysis","authors":"Jueun Kim, Simin Sun, Donghyeon Kim, Byung Gwan Park, Hojeong Lee, Wenyu Huang, Kwangjin An","doi":"10.1016/j.checat.2024.101076","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101076","url":null,"abstract":"<p>The increasing amount of plastic waste poses serious environmental problems that threaten both ecosystems and human well-being. Hydrogenolysis has been widely studied as an effective approach for converting polyolefins into high-value liquids and waxy fuels. Their multifaceted reaction mechanism, including dehydrogenation, C–C bond cleavage, and hydrogenation, highlights the need for sophisticated catalyst design. The suppression of methane production, a persistent challenge in polyolefin hydrogenolysis, requires precise control of the cleavage site and inhibition of successive C–C bond cleavage. This delicate balance is achieved by carefully tuning the size and structure of metals. In this review, we investigate the effects of the size and structure of active sites on their catalytic activity and selectivity for the hydrogenolysis of polyolefins, including polyethylene and polypropylene. A fundamental understanding of hydrogenolysis mechanisms, combined with strategic synthetic methodologies, is crucial for creating efficient catalysts with tailored properties.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Plasmon-induced photocatalytic nitrogen fixation on medium-spin Au3Fe1/Mo single-atom alloy antenna reactor 中等自旋 Au3Fe1/Mo 单原子合金天线反应器上的等离子体诱导光催化固氮作用
IF 9.4
Chem Catalysis Pub Date : 2024-08-20 DOI: 10.1016/j.checat.2024.101083
Bing-Hao Wang, Biao Hu, Guang-Hui Chen, Xiong Wang, Sheng Tian, Yang Li, Xing-Sheng Hu, Huijuan Wang, Chak-Tong Au, Li-Long Jiang, Lang Chen, Shuang-Feng Yin
{"title":"Plasmon-induced photocatalytic nitrogen fixation on medium-spin Au3Fe1/Mo single-atom alloy antenna reactor","authors":"Bing-Hao Wang, Biao Hu, Guang-Hui Chen, Xiong Wang, Sheng Tian, Yang Li, Xing-Sheng Hu, Huijuan Wang, Chak-Tong Au, Li-Long Jiang, Lang Chen, Shuang-Feng Yin","doi":"10.1016/j.checat.2024.101083","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101083","url":null,"abstract":"<p>Developing photocatalysts with active sites that have appropriate interactions with both N<sub>2</sub> and reactive intermediates has proved to be feasible for direct nitrogen reduction but is still a formidable challenge. Herein, a medium-spin Au<sub>3</sub>Fe<sub>1</sub>/Mo single-atom alloy photocatalyst with optical antenna structure is fabricated through an alloying strategy. Fe atoms of a medium-spin state anchored on Au nanoparticles at the single-atom level via Au–Fe bonding is confirmed by combined characterizations of aberration-corrected high-angle annular dark field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray absorption fine structure (XAFS), and Mössbauer spectroscopic techniques. With strong Mo-Fe-Au electronic interactions, the Fe sites act as intrinsic centers apt for nitrogen adsorption and activation, which is conducive to the preferential cleavage of the N≡N bond and modulate adsorption of reactive intermediates. Due to synergistic effect of Au nanoparticles acting as optical antennae, the Au<sub>3</sub>Fe<sub>1</sub>/Mo photocatalyst showed excellent photocatalytic nitrogen reduction reaction (pNRR) performance, giving an ammonia formation rate of 484.2 μmol h<sup>−1</sup> g<sup>−1</sup> and solar-to-ammonia (STA) conversion efficiency up to 0.12%.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Personalized machine learning models of terminal olefin hydroformylation for regioselectivity prediction 用于区域选择性预测的末端烯烃加氢甲酰化个性化机器学习模型
IF 9.4
Chem Catalysis Pub Date : 2024-08-20 DOI: 10.1016/j.checat.2024.101079
Hao Wang, Yuzhuo Chen, Hang Yu, Menghui Qi, De Xia, Minkai Qin, XuCheng Lv, Bing Lu, Ruiliang Gao, Yong Wang, Shanjun Mao
{"title":"Personalized machine learning models of terminal olefin hydroformylation for regioselectivity prediction","authors":"Hao Wang, Yuzhuo Chen, Hang Yu, Menghui Qi, De Xia, Minkai Qin, XuCheng Lv, Bing Lu, Ruiliang Gao, Yong Wang, Shanjun Mao","doi":"10.1016/j.checat.2024.101079","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101079","url":null,"abstract":"<p>The integration of machine learning into hydroformylation processes represents a pivotal advancement in high-throughput screening within the chemical industry. This study employs a data-driven approach to develop predictive models for terminal olefin reactions. Using a database of 1,167 entries, we merged reaction embeddings with corresponding labels. The well-trained extreme gradient boosting model achieves a test set coefficient of determination (R<sup>2</sup>) score of 0.897. However, when applied to specific-olefin tasks, the model shows suboptimal performance. Therefore, tailored models for specific olefins like 1-octene and styrene are developed, achieving improved test set R<sup>2</sup> scores of 0.850 and 0.789, respectively, compared to the general-olefin task. Interpretability findings highlight the significance of high-temperature, low-pressure, and low-concentration metals in enhancing linear regioselectivity and providing chemical insights. This study underscores the transformative potential of machine learning as a surrogate model in advancing high-throughput screening and optimizing chemical processes in the industry.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023112","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ti3+ sites for photocatalytic NO decomposition under visible light 可见光下光催化分解 NO 的 Ti3+ 位点
IF 9.4
Chem Catalysis Pub Date : 2024-08-15 DOI: 10.1016/j.checat.2024.101080
Chenlu Xie
{"title":"Ti3+ sites for photocatalytic NO decomposition under visible light","authors":"Chenlu Xie","doi":"10.1016/j.checat.2024.101080","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101080","url":null,"abstract":"<p>In this issue of <em>Chem Catalysis</em>, Choi and co-worker report a Ti<sup>3+</sup>-rich mesoporous TiO<sub>2-x</sub> catalyst that achieves superior performance in NO decomposition into N<sub>2</sub> and O<sub>2</sub> under visible light. The study highlights the crucial role of Ti<sup>3+</sup> sites in enhancing NO adsorption and promoting N–N coupling to form N<sub>2</sub>.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Redesigning microbial enzymes for sustainable chemical synthesis 为可持续化学合成重新设计微生物酶
IF 9.4
Chem Catalysis Pub Date : 2024-08-15 DOI: 10.1016/j.checat.2024.101087
John F.C. Steele, Stephen Wallace
{"title":"Redesigning microbial enzymes for sustainable chemical synthesis","authors":"John F.C. Steele, Stephen Wallace","doi":"10.1016/j.checat.2024.101087","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101087","url":null,"abstract":"<p>Here, we preview recent work by Zhang et al. on the computational redesign of an enoate reductase from <em>Heyndrickxia coagulans</em> for the improved biocatalytic reduction of <em>cis</em>,<em>cis</em>-muconic acid to adipic acid.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Phosphine ligand-dependent nickel-catalyzed regiodivergent isomerization of alkenes 膦配体依赖性镍催化的烯烃变异异构化反应
IF 9.4
Chem Catalysis Pub Date : 2024-08-15 DOI: 10.1016/j.checat.2024.101089
Jin-Ping Wang, Peng Wang
{"title":"Phosphine ligand-dependent nickel-catalyzed regiodivergent isomerization of alkenes","authors":"Jin-Ping Wang, Peng Wang","doi":"10.1016/j.checat.2024.101089","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101089","url":null,"abstract":"<p>Regioselective isomerization of alkenes enables efficient alkene preparation with 100% atom economy. In this issue of <em>Chem Catalysis</em>, Chen, Zhao, Wang, and co-workers present a Ni-catalyzed method for producing kinetic and thermodynamic products with high yields and excellent regioselectivity, highlighting the phosphine ligand’s role in controlling regioselectivity.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142023071","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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