Shuo Zhang, Jun Yang, Xin Cao, Hui Zhang, Yuhang Zhao, Yuying Huang, Jianhua Sun
In poly(heptazine imide) (PHI), in situ incorporated alkali metal ions are demonstrated to guide the arrangement of the PHI framework, regulate its electronic structure, modulate charge-carrier transfer, and ultimately govern the photocatalytic performance. Notably, some of the resulting structural features and properties are retained even after the removal of these cations.
{"title":"Ultrafast carrier transfer in poly(heptazine imide) for efficient photocatalytic H<sub>2</sub>O<sub>2</sub> production: the structure-directing role of <i>in situ</i> incorporated cations.","authors":"Shuo Zhang, Jun Yang, Xin Cao, Hui Zhang, Yuhang Zhao, Yuying Huang, Jianhua Sun","doi":"10.1039/d6cc00105j","DOIUrl":"10.1039/d6cc00105j","url":null,"abstract":"<p><p>In poly(heptazine imide) (PHI), <i>in situ</i> incorporated alkali metal ions are demonstrated to guide the arrangement of the PHI framework, regulate its electronic structure, modulate charge-carrier transfer, and ultimately govern the photocatalytic performance. Notably, some of the resulting structural features and properties are retained even after the removal of these cations.</p>","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":" ","pages":"6328-6331"},"PeriodicalIF":4.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147363556","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Optimizing the adsorption of oxygen-containing intermediates by regulating the electronic structure to enhance the oxygen reduction reaction(ORR) activity of catalysts is crucial. In this article, the coupled effects of tensile strain and atomic-scale cavity (ASC) defects on the ORR activity of a d-PdW bimetallene are investigated. The d-PdW exhibits excellent ORR performance with a half-wave potential as high as 0.96 V (vs. RHE) and mass activity of 5.2 A mgcatalyst-1 at 0.9 V. X-ray absorption characterizations and DFT calculations were used to explain the reasons for the good performance.
通过调节电子结构来优化含氧中间体的吸附，提高催化剂的氧还原反应活性是至关重要的。本文研究了拉伸应变和原子尺度空腔缺陷对d-PdW双金属烯ORR活性的耦合影响。d-PdW表现出优异的ORR性能，半波电位高达0.96 V（相对于RHE）， 0.9 V时质量活性为5.2 a mgcatalyst-1。利用x射线吸收特性和DFT计算来解释良好性能的原因。
{"title":"Uncovering the effect of lattice strain and atomic-scale cavity deficiency on the efficient oxygen reduction of a PdW bimetallene.","authors":"Jigang Wang, Xia Zhou, Yinggang Sun, Xiuhui Bai, Lancheng Zhao, Siqi Wang, Likai Wang, Huan Liu, Zhongfang Li","doi":"10.1039/d5cc06989k","DOIUrl":"10.1039/d5cc06989k","url":null,"abstract":"<p><p>Optimizing the adsorption of oxygen-containing intermediates by regulating the electronic structure to enhance the oxygen reduction reaction(ORR) activity of catalysts is crucial. In this article, the coupled effects of tensile strain and atomic-scale cavity (ASC) defects on the ORR activity of a d-PdW bimetallene are investigated. The d-PdW exhibits excellent ORR performance with a half-wave potential as high as 0.96 V (<i>vs.</i> RHE) and mass activity of 5.2 A mg<sub>catalyst</sub><sup>-1</sup> at 0.9 V. X-ray absorption characterizations and DFT calculations were used to explain the reasons for the good performance.</p>","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":" ","pages":"6382-6386"},"PeriodicalIF":4.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147375439","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kai Chen,Guangda Han,Sunny Yadav,Jinquan Li,Vandung Dao,Periyayya Uthirakumar,In-Hwan Lee
Single-atom catalysis (SACs) has attracted considerable attention because of its distinctive structural characteristics and strong potential for catalytic innovation. The performance of atomically dispersed catalysts depends on the local microenvironment surrounding the single atoms and neighboring active species. Moreover, the local microenvironment constrains the electronic structure and geometry of the catalyst, thereby determining the efficiency of the energy-conversion devices. However, significant challenges persist in accurately designing the electronic coordination environments and geometric configurations of catalysts at the sub-nanometer scale, which limits effective regulation of the catalytic microenvironment and improvement of catalytic activity. This review provides a comprehensive overview of the cutting-edge progress in enhancing energy conversion efficiency via micro-environmental regulation of single-atom catalysts. Typical techniques for regulating local coordination microenvironments are discussed, including heterogeneous atom anchoring, atomic molecular bridging, defect engineering, spatial confinement, and construction of local microinterfaces. Characterization techniques for probing microenvironments, such as X-ray absorption fine structure spectroscopy, are also summarized. The optimization of single-atom efficiency via local microenvironment regulation has been demonstrated for the HER, OER, ORR, CO2RR, and NRR. The discussion concludes with an assessment of application prospects and remaining challenges associated with engineering-based microenvironment control, aiming to guide future developments in single-atom precision catalysis and energy conversion devices.
{"title":"Adjusting the local coordination microenvironment of single atoms to optimize catalytic efficiency in renewable energy devices.","authors":"Kai Chen,Guangda Han,Sunny Yadav,Jinquan Li,Vandung Dao,Periyayya Uthirakumar,In-Hwan Lee","doi":"10.1039/d6cc00260a","DOIUrl":"https://doi.org/10.1039/d6cc00260a","url":null,"abstract":"Single-atom catalysis (SACs) has attracted considerable attention because of its distinctive structural characteristics and strong potential for catalytic innovation. The performance of atomically dispersed catalysts depends on the local microenvironment surrounding the single atoms and neighboring active species. Moreover, the local microenvironment constrains the electronic structure and geometry of the catalyst, thereby determining the efficiency of the energy-conversion devices. However, significant challenges persist in accurately designing the electronic coordination environments and geometric configurations of catalysts at the sub-nanometer scale, which limits effective regulation of the catalytic microenvironment and improvement of catalytic activity. This review provides a comprehensive overview of the cutting-edge progress in enhancing energy conversion efficiency via micro-environmental regulation of single-atom catalysts. Typical techniques for regulating local coordination microenvironments are discussed, including heterogeneous atom anchoring, atomic molecular bridging, defect engineering, spatial confinement, and construction of local microinterfaces. Characterization techniques for probing microenvironments, such as X-ray absorption fine structure spectroscopy, are also summarized. The optimization of single-atom efficiency via local microenvironment regulation has been demonstrated for the HER, OER, ORR, CO2RR, and NRR. The discussion concludes with an assessment of application prospects and remaining challenges associated with engineering-based microenvironment control, aiming to guide future developments in single-atom precision catalysis and energy conversion devices.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"12 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yi Wang,Qi Qian,Zehua Zou,Xuan Zheng,Qinghua Wang,Yun Ling,Qingxiang Wang
Li+ leaching triggers electrochemical reconstruction of Li4Ti5O12 spinel into TiO2 rutile on Ti foil. This phase transformation preserves structural integrity, enabling stable H2O2 production at 74.69 µM h-1 cm-2 for 120 hours in acidic electrolyte through 2e- water oxidation.
{"title":"Lithium-induced reconstruction of Li4Ti5O12 for acidic H2O2 production via two-electron water oxidation.","authors":"Yi Wang,Qi Qian,Zehua Zou,Xuan Zheng,Qinghua Wang,Yun Ling,Qingxiang Wang","doi":"10.1039/d6cc00997b","DOIUrl":"https://doi.org/10.1039/d6cc00997b","url":null,"abstract":"Li+ leaching triggers electrochemical reconstruction of Li4Ti5O12 spinel into TiO2 rutile on Ti foil. This phase transformation preserves structural integrity, enabling stable H2O2 production at 74.69 µM h-1 cm-2 for 120 hours in acidic electrolyte through 2e- water oxidation.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"19 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502491","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anup Kumar Mondal, D. Srinivasa Reddy, Dattatraya P Masal
Herein, we report the first total synthesis of (±)-Cyclopeltain B, a structurally unique alkylated adenine derivative featuring a rare 6/5/7/5 fused ring system. The synthesis was accomplished using commercially available adenine and (Z)-but-2ene-1,4-diol as starting materials. Key steps include an Aza-Michael addition followed by a TiCl4-mediated one-pot five-step cascade reaction to construct the complex (6/5/7/5) fused ring scaffold. The structure of the synthetic (±)-Cyclopeltain B was confirmed by X-ray crystallographic analysis in addition to spectral data comparison with the natural product. Furthermore, a series of structurally related analogues was synthesised to evaluate their biological activities.
{"title":"Total Synthesis of (±)-Cyclopeltain B","authors":"Anup Kumar Mondal, D. Srinivasa Reddy, Dattatraya P Masal","doi":"10.1039/d6cc00023a","DOIUrl":"https://doi.org/10.1039/d6cc00023a","url":null,"abstract":"Herein, we report the first total synthesis of (±)-Cyclopeltain B, a structurally unique alkylated adenine derivative featuring a rare 6/5/7/5 fused ring system. The synthesis was accomplished using commercially available adenine and (Z)-but-2ene-1,4-diol as starting materials. Key steps include an Aza-Michael addition followed by a TiCl4-mediated one-pot five-step cascade reaction to construct the complex (6/5/7/5) fused ring scaffold. The structure of the synthetic (±)-Cyclopeltain B was confirmed by X-ray crystallographic analysis in addition to spectral data comparison with the natural product. Furthermore, a series of structurally related analogues was synthesised to evaluate their biological activities.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"1 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bifu Liu, Qiaoya Zhang, Jun Zhang, Aidong Huang, Hulin Zhong, Kejun Feng, Yang Gao, Yanping Huo, Qian Chen, Xianwei Li
A weakly coordinating amide-directed C-H alkynylation enables late-stage modification of complex drug and material analogues bearing multiple reactive C-H bonds. This approach achieves divergent regioselectivity in celecoxib and valdecoxib derivatives that contained strongly coordinating heterocycles, by exploiting complementary reactivity between amide substrates, metal catalysts, and haloalkyne coupling partners.
{"title":"Tunable regioselectivity for C-H alkynylation of weakly coordinating amides that tolerated strongly coordinating heterocycles.","authors":"Bifu Liu, Qiaoya Zhang, Jun Zhang, Aidong Huang, Hulin Zhong, Kejun Feng, Yang Gao, Yanping Huo, Qian Chen, Xianwei Li","doi":"10.1039/d6cc00867d","DOIUrl":"10.1039/d6cc00867d","url":null,"abstract":"<p><p>A weakly coordinating amide-directed C-H alkynylation enables late-stage modification of complex drug and material analogues bearing multiple reactive C-H bonds. This approach achieves divergent regioselectivity in celecoxib and valdecoxib derivatives that contained strongly coordinating heterocycles, by exploiting complementary reactivity between amide substrates, metal catalysts, and haloalkyne coupling partners.</p>","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":" ","pages":"6373-6377"},"PeriodicalIF":4.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147363579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
An unprecedented catalyst-free cyclization reaction of easily accessed enynone and unprotected hydrazine is reported. Featuring simple reaction conditions, high efficiency and broad substrate scope, this protocol provides a practical synthetic method to access various bio-related pyrazolo[5,1-a]isoquinolines derivatives in up to 82% yields using environmentally friendly solvent EtOH under air atmosphere.
{"title":"Catalyst-free Synthesis of Pyrazolo[5,1-a]isoquinolines from Hydrazine Hydrate","authors":"Yangxin Mao, Shaotong Qiu, Xinlei Wang, Yimin Shangguan, Jiangan Liu, Zhicheng Yang, Yun-Hui Zhao, Xiaofang Li, Baishu Zheng, Hu Zhou","doi":"10.1039/d6cc00525j","DOIUrl":"https://doi.org/10.1039/d6cc00525j","url":null,"abstract":"An unprecedented catalyst-free cyclization reaction of easily accessed enynone and unprotected hydrazine is reported. Featuring simple reaction conditions, high efficiency and broad substrate scope, this protocol provides a practical synthetic method to access various bio-related pyrazolo[5,1-a]isoquinolines derivatives in up to 82% yields using environmentally friendly solvent EtOH under air atmosphere.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"15 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496393","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Haohong Xian, hong tang, Keying Zhong, Jiaqian Liu, Haoran Guo, Haibing Wei, Tingshuai Li
Seawater electrolysis is emerging as a compelling route for green hydrogen production, but its practical implementation is severely limited by chloride-induced corrosion. Herein, we report a sulfate-intercalated NiFe layered double hydroxide on nickel foam (S-NiFe LDH/NF) as a scalable and efficient electrocatalyst for alkaline seawater oxidation (ASO), which achieves 1 A cm−2 with a low overpotential of 375 mV and exhibits remarkable stability for 1800 h at this current density. MEA testing further confirms its durability, showing stable operation over 200 h at 500 mA cm−2. In situ Raman spectroscopy characterization and stability tests indicate that sulfate accelerates the formation of catalytically active γ-NiOOH and effectively repels chloride ion.
海水电解正在成为一种引人注目的绿色制氢途径，但其实际实施受到氯化物引起的腐蚀的严重限制。在此，我们报道了一种硫酸盐插层NiFe层状双氢氧化物泡沫镍（S-NiFe LDH/NF）作为可扩展和高效的碱性海水氧化（ASO）电催化剂，其电流密度为1 a cm - 2，过电位为375 mV，并在该电流密度下表现出1800 h的显著稳定性。MEA测试进一步证实了其耐久性，在500毫安厘米−2下稳定运行200小时。原位拉曼光谱表征和稳定性测试表明，硫酸盐加速了催化活性γ-NiOOH的形成，并有效地排斥氯离子。
{"title":"Scalable NiFe layered double hydroxides for efficient electrocatalytic seawater oxidation at high current density","authors":"Haohong Xian, hong tang, Keying Zhong, Jiaqian Liu, Haoran Guo, Haibing Wei, Tingshuai Li","doi":"10.1039/d5cc07357j","DOIUrl":"https://doi.org/10.1039/d5cc07357j","url":null,"abstract":"Seawater electrolysis is emerging as a compelling route for green hydrogen production, but its practical implementation is severely limited by chloride-induced corrosion. Herein, we report a sulfate-intercalated NiFe layered double hydroxide on nickel foam (S-NiFe LDH/NF) as a scalable and efficient electrocatalyst for alkaline seawater oxidation (ASO), which achieves 1 A cm−2 with a low overpotential of 375 mV and exhibits remarkable stability for 1800 h at this current density. MEA testing further confirms its durability, showing stable operation over 200 h at 500 mA cm−2. In situ Raman spectroscopy characterization and stability tests indicate that sulfate accelerates the formation of catalytically active γ-NiOOH and effectively repels chloride ion.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"92 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Here we present copper sulfide-promoted urea nitrosylation as a nonenzymatic means of carbamoylation, demonstrating a variety of prebiotically important reactions, including the formation of carbamoyl phosphate from urea and phosphate, the phosphorylation of uridine to uridine monophosphate, and the carbamoylation of aspartate at 25°C and pH 6–7.
{"title":"Nonenzymatic Carbamoylation and Phosphorylation via Urea Nitrosylation under Mild Aqueous Conditions","authors":"Nishiki Tomizawa, Norio Kitadai, Shotaro Tagawa, Ryuhei Nakamura","doi":"10.1039/d5cc05999b","DOIUrl":"https://doi.org/10.1039/d5cc05999b","url":null,"abstract":"Here we present copper sulfide-promoted urea nitrosylation as a nonenzymatic means of carbamoylation, demonstrating a variety of prebiotically important reactions, including the formation of carbamoyl phosphate from urea and phosphate, the phosphorylation of uridine to uridine monophosphate, and the carbamoylation of aspartate at 25°C and pH 6–7.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"14 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A S/NiMoSe hierarchical microsphere-supported nanofiber electrocatalyst was synthesized via a surface sulfidation strategy. It exhibits excellent alkaline HER performance: -69 mV overpotential at -10 mA cm-2 and 41 h durability at -100 mA cm-2. Surface sulfidation weakens interfacial water hydrogen-bonding and gene-rates SO42- via reconstruction, thus sustaining high electrocatalyst activity and stability.
采用表面硫化法制备了S/NiMoSe层次化微球负载纳米纤维电催化剂。它具有优异的碱性HER性能：在-10 mA cm-2下的过电位为-69 mV，在-100 mA cm-2下的耐久性为41 h。表面硫化通过重构削弱界面水氢键和SO42-基因速率，从而保持较高的电催化剂活性和稳定性。
{"title":"Surface sulfidation toward highly active S/NiMoSe for superior alkaline hydrogen evolution","authors":"Xinyu Li, Huaiqing Yan, Yue Xiao, Fuxi Bao, Wen Guo","doi":"10.1039/d6cc00626d","DOIUrl":"https://doi.org/10.1039/d6cc00626d","url":null,"abstract":"A S/NiMoSe hierarchical microsphere-supported nanofiber electrocatalyst was synthesized via a surface sulfidation strategy. It exhibits excellent alkaline HER performance: -69 mV overpotential at -10 mA cm-2 and 41 h durability at -100 mA cm-2. Surface sulfidation weakens interfacial water hydrogen-bonding and gene-rates SO42- via reconstruction, thus sustaining high electrocatalyst activity and stability.","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":"59 1","pages":""},"PeriodicalIF":4.9,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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