Chem Catalysis最新文献_第10页

Engineering intricacies of implementing single-atom alloy catalysts for low-temperature electrocatalytic CO2 reduction 实施单原子合金催化剂用于低温电催化二氧化碳还原的工程复杂性

IF 9.4

Chem Catalysis Pub Date : 2024-10-29 DOI: 10.1016/j.checat.2024.101164

Isaac Kojo Seim, Manjeet Chhetri, John-Paul Jones, Ming Yang

{"title":"Engineering intricacies of implementing single-atom alloy catalysts for low-temperature electrocatalytic CO2 reduction","authors":"Isaac Kojo Seim, Manjeet Chhetri, John-Paul Jones, Ming Yang","doi":"10.1016/j.checat.2024.101164","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101164","url":null,"abstract":"Catalysts research for electrocatalytic CO2 reduction reactions (CO2R) has undergone rapid growth in the last decade. Single-atom alloy catalysts (SAAs) featuring atomically dispersed metal dopants on host metal surfaces have shown promises in boosting CO2R yield by optimizing the structure and synergy of the catalytic metals at the atomic scale. Despite the exciting development of SAAs for CO2R in fundamental science, dedicated studies for its engineering implementation have been absent. We use this perspective to discuss our non-exhaustive engineering considerations for implementing SAAs for CO2R. The perspective starts with a brief overview of the current research status for SAAs in CO2R, followed by focal points on structure uncertainties associated with catalyst manufacturing, catalyst layer degradation during reaction, and possibilities for SAAs to mitigate the salt precipitation issue at the device level. We hope our opinions will engage increasing attention toward the engineering catalysis research for applying SAAs to CO2R at scale.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142536538","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

Discrimination between OH− and H2O oxidation for oxygen evolution reaction 区分氧进化反应中的 OH- 氧化和 H2O 氧化

IF 9.4

Chem Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.checat.2024.101157

Mengjun Xiao, Qianbao Wu, Hongfei Liu, Xia Zheng, Lei Li, Wei Wang, Chunhua Cui

{"title":"Discrimination between OH− and H2O oxidation for oxygen evolution reaction","authors":"Mengjun Xiao, Qianbao Wu, Hongfei Liu, Xia Zheng, Lei Li, Wei Wang, Chunhua Cui","doi":"10.1016/j.checat.2024.101157","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101157","url":null,"abstract":"OH−/H2O-reactant discrimination for the oxygen evolution reaction (OER) is a critical but not well resolved issue. This has led to unreasonable activity comparisons, misinterpreted OER mechanisms, and ununified models for theoretical calculations regardless of the thermodynamic/kinetic difference between OH− and H2O oxidation. Here, we discriminate between OH− and H2O oxidation by tuning the interfacial OH− concentration. Combining OER kinetic analysis with in situ 16OH−/H218O isotopic labeling-based differential electrochemical mass spectrometry, we examine the respective electrochemical oxidation behaviors between OH− and H2O oxidation. We find that OH− oxidation presents ∼550 mV lower onset potential relative to H2O oxidation and that Tafel plotting gives slopes of ∼50 mV dec−1 for OH− oxidation, which is substantially lower than those of ∼200 mV dec−1 for H2O oxidation on a model CoOOH catalyst. This work calls for the discrimination of OH−/H2O oxidation as the prerequisite for future OER activity evaluation and mechanism studies.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"49 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519379","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

An electrocatalytic oxidative approach to synthesis urea 电催化氧化法合成尿素

IF 9.4

Chem Catalysis Pub Date : 2024-10-28 DOI: 10.1016/j.checat.2024.101181

Shuangyin Wang

引用次数: 0

Practical and modular cycloadditions of in-situ formed exocyclic vinylcarbenes 原位形成外环乙烯基烯烃的实用模块化环化反应

IF 9.4

Chem Catalysis Pub Date : 2024-10-25 DOI: 10.1016/j.checat.2024.101163

Cheng Zhang, Shanliang Dong, Martin C. Dietl, Matthias Rudolph, Xinke Zhang, Kemiao Hong, Wei Yi, A. Stephen K. Hashmi, Xinfang Xu

引用次数: 0

Boosting photocatalytic water oxidation on lead chromate through crystal facet engineering 通过晶面工程提高铬酸铅的光催化水氧化能力

IF 9.4

Chem Catalysis Pub Date : 2024-10-25 DOI: 10.1016/j.checat.2024.101153

Wenchao Jiang, Chenwei Ni, Yejun Xiao, Yue Zhao, Chu Han, Xuan Wu, Chengbo Zhang, Haibo Chi, Rengui Li, Can Li

{"title":"Boosting photocatalytic water oxidation on lead chromate through crystal facet engineering","authors":"Wenchao Jiang, Chenwei Ni, Yejun Xiao, Yue Zhao, Chu Han, Xuan Wu, Chengbo Zhang, Haibo Chi, Rengui Li, Can Li","doi":"10.1016/j.checat.2024.101153","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101153","url":null,"abstract":"Although crystal facet engineering of semiconductor crystals has been demonstrated to be effective in particulate photocatalysts for solar energy conversion, it is imperative to rationally regulate the exposed crystal facets and their configurations to improve charge separation efficiency. In this study, focusing on visible-light-driven water oxidation photocatalyst lead chromate (PbCrO4), we find that a flux-assisted treatment enables the precise tuning of the hole-accumulating facets of anisotropic PbCrO4 crystal, transitioning the top surface from {−101} to {001} facets while preserving its spatial charge separation characteristics. Owing to the superior hole-accumulating property and water oxidation kinetics of the {001} facets, the resulting Flux-PbCrO4 crystals achieve a charge separation efficiency exceeding 75%, leading to a remarkable improvement in photocatalytic water oxidation activity. Further incorporation of cocatalysts onto the Flux-PbCrO4 crystals results in an apparent quantum efficiency of 18.5% at 500 nm for photocatalytic water oxidation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"6 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489834","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

Expanding the repertoire of imine reductases by mining divergent biosynthetic pathways for promiscuous reactivity 通过挖掘不同生物合成途径的杂合反应性，扩大亚胺还原酶的范围

IF 9.4

Chem Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.checat.2024.101160

Godwin A. Aleku, Florian Hollfelder

引用次数: 0

Ketones as ideal photocatalysts for decarboxylative fluorination and a competition with C(sp3)-H fluorination 酮类作为理想的光催化剂用于脱羧氟化以及与 C（sp3）-H 氟化的竞争

IF 9.4

Chem Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.checat.2024.101162

Yu Zhang, Jiahui Qian, Miao Wang, Yahao Huang, Hansjörg Grützmacher, Peng Hu

引用次数: 0

Photoreduction of CO2 to complete CO catalyzed by charge-density-regulating metal-organic frameworks 在电荷密度调节金属有机框架催化下将 CO2 光还原为完全 CO

IF 9.4

Chem Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.checat.2024.101154

Luyao Wang, Yifan Gu, Fengting Li

{"title":"Photoreduction of CO2 to complete CO catalyzed by charge-density-regulating metal-organic frameworks","authors":"Luyao Wang, Yifan Gu, Fengting Li","doi":"10.1016/j.checat.2024.101154","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101154","url":null,"abstract":"Photoreduction of CO2 to a single gas product requires catalysts with remarkable product selectivity because CO and CH4 are usually produced simultaneously. We propose that the charge-density regulation within metal-organic frameworks (MOFs) could effectively manage the binding energy required for reduction intermediates, thereby controlling the ultimate product formation to obtain CO with 100% selectivity. Herein, two iso-structured Fe-based MOFs bearing linkers with different electronic properties were prepared and exhibited favorable CO2 photoreduction performance without any cocatalyst or photosensitizer. In particular, the linker was altered to reduce the transfer of charges from Fe to the surrounding ligands, regulating the charge-density distribution. The binding affinity with the key COH∗ was remarkably weakened and behaved thermodynamically unfavorably compared with CO desorption, resulting in 100% CO generation. These insights provide a catalyst design strategy for controlling reduction species and improving product selectivity, which could encourage the development of intriguing MOF material customization for photocatalysis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489082","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

Fine-tuning catalytic selectivity by modulating catalyst-environment interactions: CO2 hydrogenation over Pd-based catalysts 通过调节催化剂与环境的相互作用微调催化选择性：钯基催化剂的二氧化碳加氢反应

IF 9.4

Chem Catalysis Pub Date : 2024-10-22 DOI: 10.1016/j.checat.2024.101156

Hong Zhang, Ping Liu

{"title":"Fine-tuning catalytic selectivity by modulating catalyst-environment interactions: CO2 hydrogenation over Pd-based catalysts","authors":"Hong Zhang, Ping Liu","doi":"10.1016/j.checat.2024.101156","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101156","url":null,"abstract":"Capturing catalytic behaviors under operational conditions is pivotal to gaining a mechanistic understanding and promoting the design of robust catalysts. The challenge lies in the difficulty of monitoring real-time surface dynamics driven by catalyst-environment interactions. Here, we introduce a framework based on density functional calculations and kinetic modeling. This framework significantly improves the accuracy of theoretical models’ descriptions of experimental observations by quantifying environmental impacts on surface phases and active sites. CO2 hydrogenation over Pd-based catalysts is taken as a showcase. The observed selectivity variations of Pd and Pd-M bimetallic catalysts strongly correlate with hydrogen coverage maintained under typical CO2 hydrogenation conditions. By reducing the amount of surface hydrogen, the selectivity tuned effectively from formic acid toward CO and methanol. This study not only deepens the comprehension of dynamics of active sites under active chemical conditions but also introduces an alternative opportunity for catalytic tuning by modulating catalyst-environment interactions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"75 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486571","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

Electrochemical CO2 fixation with amines to synthesize α-amino acids 用胺进行电化学二氧化碳固定以合成α-氨基酸

IF 9.4

Chem Catalysis Pub Date : 2024-10-22 DOI: 10.1016/j.checat.2024.101158

Yimeng Cao, Jun Chen, Chunmei Ding, Ying Zhang, Haibo Chi, Yan Liu, Can Li

引用次数: 0