Research on Chemical Intermediates最新文献

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Efficient and stable synthesis of diethylene glycol dimethyl ether over aluminophosphate catalyst 磷酸铝催化高效稳定合成二甘醇二甲醚
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-07-01 DOI: 10.1007/s11164-025-05667-5
Zhichuang Li, Jingchen Wu, Xiujing Zou, Xingfu Shang, Xueguang Wang
{"title":"Efficient and stable synthesis of diethylene glycol dimethyl ether over aluminophosphate catalyst","authors":"Zhichuang Li,&nbsp;Jingchen Wu,&nbsp;Xiujing Zou,&nbsp;Xingfu Shang,&nbsp;Xueguang Wang","doi":"10.1007/s11164-025-05667-5","DOIUrl":"10.1007/s11164-025-05667-5","url":null,"abstract":"<div><p>A series of aluminophosphate catalysts (<i>x</i>P-Al-O-<i>T</i>) with various P/Al molar ratios and calcination temperatures were prepared through a one-pot reaction with F127. The physical and chemical properties of the prepared<i> x</i>P-Al-O-<i>T</i> catalysts were thoroughly investigated using methods such as XRD, FTIR, Py-FTIR, low-temperature nitrogen adsorption–desorption, and NH₃-TPD. The results showed that the prepared <i>x</i>P-Al-O-<i>T</i> samples existed in the amorphous form and weak Lewis acidic sites on the surfaces were predominant. The prepared catalysts were investigated for their catalytic behaviors in gas-phase etherification of diethylene glycol monomethyl ether (DEGME) with dimethyl carbonate (DMC) to produce diethylene glycol dimethyl ether (DEGDME), which is regarded as a green synthetic route. The effects of different P/Al molar ratios and calcination temperatures on the catalyst performance were studied. All the tested catalysts exhibited 100% DEGME conversion. When the calcination temperature was 550 °C and the P/Al molar ratio was 0.75, the aluminophosphate catalyst could proceed for 248 h without significant loss of activity and changes in product DEGDME selectivity, showing the long catalytic stability.</p><h3>Graphical abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 9","pages":"4937 - 4956"},"PeriodicalIF":3.5,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144918219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
An in-depth investigation for biodiesel production and Knoevenagel condensation using pineapple peels-derived eco-friendly catalyst 深入研究菠萝皮衍生的环保催化剂在生物柴油生产和Knoevenagel缩合中的应用
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-30 DOI: 10.1007/s11164-025-05660-y
Manisha Chadha, Shazia Hussain, Shiwani Berry
{"title":"An in-depth investigation for biodiesel production and Knoevenagel condensation using pineapple peels-derived eco-friendly catalyst","authors":"Manisha Chadha,&nbsp;Shazia Hussain,&nbsp;Shiwani Berry","doi":"10.1007/s11164-025-05660-y","DOIUrl":"10.1007/s11164-025-05660-y","url":null,"abstract":"<div><p>Green catalysts derived from biowastes like agricultural waste or biomass offers a sustainable option compared to catalysts obtained from commercial sources. This study emphasizes the effective synthesis of biodiesel production and Knoevenagel condensation using a sustainable catalyst derived from pineapple peels. The catalyst underwent characterization through a variety of techniques including Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), field emission-scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HR-TEM), Brunauer–Emmett–Teller (BET), thermogravimetric analysis (TGA), and energy-dispersive X-ray (EDX) methods. The catalyst's active sites consist of alkali metal oxides, hydroxides, and carbonates, which are essential for the formation of the desired products. The biodiesel was formed with high percentage conversion rate of 97.5%; however, Knoevenagel products were synthesized with an extremely high percentage yield, i.e. up to 96%. In addition, the products underwent characterization using <sup>1</sup>H and <sup>13</sup>C nuclear magnetic resonance spectra. The study delved into the reusability and stability of the catalyst, showing the recyclability of up to four cycles with 79% yield, revealing encouraging results for potential industrial applications.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4281 - 4314"},"PeriodicalIF":3.5,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171750","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sustainable Knoevenagel condensation catalyzed by recyclable biopolymer under concentrated solar radiation 聚光辐射下可回收生物聚合物催化的可持续Knoevenagel缩合反应
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-30 DOI: 10.1007/s11164-025-05673-7
Santosh S. Chikane, Dipak V. Pinjari, Pranit B. Patil, Bharat G. Pawar, Nitin D. Arote
{"title":"Sustainable Knoevenagel condensation catalyzed by recyclable biopolymer under concentrated solar radiation","authors":"Santosh S. Chikane,&nbsp;Dipak V. Pinjari,&nbsp;Pranit B. Patil,&nbsp;Bharat G. Pawar,&nbsp;Nitin D. Arote","doi":"10.1007/s11164-025-05673-7","DOIUrl":"10.1007/s11164-025-05673-7","url":null,"abstract":"<div><p>A sustainable Knoevenagel condensation protocol using recyclable chitosan as a biopolymer-based catalyst under concentrated solar radiation (CSR) has been developed. This green method eliminates conventional heating and harsh reagents by utilizing CSR as a renewable energy source. The catalyst is easily recoverable and reusable across multiple cycles with minimal activity loss, ensuring both environmental and economic advantages. The approach offers high yields (up to 98%) within short reaction times (8–28 min), demonstrating excellent atom economy and energy efficiency (89–99%) in alignment with green chemistry principles.</p><h3>Graphical abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4261 - 4279"},"PeriodicalIF":3.5,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145171749","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Outperformance of CaO-incorporated alumina-supported Pd catalysts in methanol decomposition cao掺杂铝负载Pd催化剂在甲醇分解中的优异性能
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-27 DOI: 10.1007/s11164-025-05652-y
Busra Eryildirim, Nuray Oktar, Doruk Dogu
{"title":"Outperformance of CaO-incorporated alumina-supported Pd catalysts in methanol decomposition","authors":"Busra Eryildirim,&nbsp;Nuray Oktar,&nbsp;Doruk Dogu","doi":"10.1007/s11164-025-05652-y","DOIUrl":"10.1007/s11164-025-05652-y","url":null,"abstract":"<div><p>This study aimed to investigate the impact of CaO incorporation to alumina-supported Pd catalysts on the methanol decomposition reaction. For this purpose, mayenite, alumina and/or calcium oxide-supported Pd catalysts were synthesized. The synthesized catalysts were characterized by XRD, FTIR, Laser Raman spectroscopy, N<sub>2</sub> adsorption–desorption, pyridine adsorbed DRIFTS, CO<sub>2</sub>-TPD, XPS, SEM–EDS, and ICP-OES techniques. Catalytic activity tests were carried out over a 6 h reaction period in the range of 100–400 °C. The results of the characterization and activity tests showed that the addition of CaO had significant effects on the physicochemical properties of the catalyst as well as on the catalytic activity. By adding CaO to the alumina support material, the acidity was reduced, thus reducing the selectivity for dimethyl ether (DME) formation, which is significantly high for the 1Pd@Al<sub>2</sub>O<sub>3</sub> catalyst, and increasing the H<sub>2</sub> and CO selectivity. The mayenite-supported catalyst (1Pd@SGM), which contains alumina and calcium oxide in its unique crystal structure, showed an excellent catalytic performance close to complete methanol conversion with DME selectivity below 1% at 400 °C. In the stability test carried out at 350 °C for 6 h with 1Pd@Al<sub>2</sub>O<sub>3</sub>, 1Pd@SGM, and 1Pd@48CaO@Al<sub>2</sub>O<sub>3</sub> catalysts used in the temperature scan, it was concluded that all catalysts were stable and 1Pd@SGM catalyst showed higher catalytic activity than the others.</p><h3>Graphical abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4149 - 4176"},"PeriodicalIF":3.5,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11164-025-05652-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145169430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sulfonated hexamine ionic liquid on boehmite as a novel, robust and recoverable bifunctional catalyst in the selective oxidation of sulfides 在薄水铝石上磺化六价离子液体作为一种新型的、稳定的、可回收的双功能催化剂用于硫化物选择性氧化
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-27 DOI: 10.1007/s11164-025-05649-7
Omid Soleimani, Bahman Tahmasbi
{"title":"Sulfonated hexamine ionic liquid on boehmite as a novel, robust and recoverable bifunctional catalyst in the selective oxidation of sulfides","authors":"Omid Soleimani,&nbsp;Bahman Tahmasbi","doi":"10.1007/s11164-025-05649-7","DOIUrl":"10.1007/s11164-025-05649-7","url":null,"abstract":"<div><p>A new protocol for the chemoselective preparation of sulfoxide using sulfonated hexamine ionic liquid on boehmite (boehmite@IL–SO<sub>3</sub>H) as a novel, robust, and heterogeneous catalyst has been developed. At first, boehmite was obtained in aqueous media using available materials. In the second step, boehmite was modified by 3-iodopropyltrimethoxysilan and then was functionalized by hexamine toward the formation of supported ionic liquid on boehmite. In the third step, chlorosulfonic acid was added to synthesis boehmite@IL–SO<sub>3</sub>H as the final catalyst. The obtained catalyst was characterized using TGA, XRD, SEM, EDS, FT-IR, BET, and WDX techniques. The XRD pattern showed that the crystal structure of boehmite remained stable in boehmite@IL–SO<sub>3</sub>H after functionalization of IL–SO<sub>3</sub>H. BET analysis showed that the surface area, pore volume, and pore diameter of this catalyst were 32.344 m<sup>2</sup>/g<sup>−1</sup>, 0.1138 cm<sup>3</sup>/g<sup>−1</sup>, and 14.074 nm, respectively. The BET results indicate a type V isotherm and a type H<sub>3</sub> hysteresis loop, indicating a flaky morphology with open pores, which is specific to the boehmite structure. Also, SEM images confirmed the BET results and showed a flaky morphology and sheet structure with a thickness of less than 50 nm for boehmite@IL–SO<sub>3</sub>H. This catalyst was investigated in the selective oxidation of sulfide to sulfoxide under solvent-free conditions using H<sub>2</sub>O<sub>2</sub> as an oxidant. The synthesized sulfoxides were confirmed by NMR spectroscopy. Boehmite@IL–SO<sub>3</sub>H heterogeneous catalyst has benefits such as being cost-effective and recyclable.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4447 - 4465"},"PeriodicalIF":3.5,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145169420","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Eco-friendly Biginelli reaction via copper–chitosan catalyst 铜-壳聚糖催化的环保Biginelli反应
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-26 DOI: 10.1007/s11164-025-05645-x
Magda H. Abdellattif, Chou-Yi Hsu, Munthar Kadhim Abosaoda, Ashok Kumar Bishoyi, Suhas Ballal, Manal Morad Karim, Abhayveer Singh, S. Supriya, Rajashree Panigrahi
{"title":"Eco-friendly Biginelli reaction via copper–chitosan catalyst","authors":"Magda H. Abdellattif,&nbsp;Chou-Yi Hsu,&nbsp;Munthar Kadhim Abosaoda,&nbsp;Ashok Kumar Bishoyi,&nbsp;Suhas Ballal,&nbsp;Manal Morad Karim,&nbsp;Abhayveer Singh,&nbsp;S. Supriya,&nbsp;Rajashree Panigrahi","doi":"10.1007/s11164-025-05645-x","DOIUrl":"10.1007/s11164-025-05645-x","url":null,"abstract":"<div><p>In this study, one of the most unique green catalysts named Cu-Picolin-Chitosan-mTEG was designed, synthesized and analyzed using different methods such as XRD, FESEM, TEM, TGA, FTIR, EDX-EDS, DLS, and ICP analyses. After confirming of synthesized nanocomposite, it is tested in oxidation of various alcohols to aldehyde and the insitu formed aldehydes are condensed with thiourea and 4‑hydroxycumarin. Finally, the synthesis of nine new thioxochromenopyrimidine derivatives by Cu-Picolin-Chitosan-mTEG is examined in perfect yields from alcohol derivatives. The conditions for reaction are green, and water is used as a solvent. This protocol offers several notable advantages, such as cost-effectiveness, atom economy, low catalyst loading, green oxidants, mild conditions, high yields, and recyclability of the nanocomposite over five cycles. Notably, this is the first report on the use of this nanocomposite for the synthesis of thioxochromenopyrimidine derivatives.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 9","pages":"5059 - 5078"},"PeriodicalIF":3.5,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144918628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Regulating the redox sites of MMoOx (M = Mn, Fe, Cr) catalysts for highly efficient selective catalytic oxidation of NH3 调节MMoOx (M = Mn, Fe, Cr)催化剂的氧化还原位点对NH3的高效选择性催化氧化
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-26 DOI: 10.1007/s11164-025-05651-z
Lan Hu, Qiuyue Zhao, Xinling Zhang, Huipeng Li, Cheng Bian, Yiqing Zeng
{"title":"Regulating the redox sites of MMoOx (M = Mn, Fe, Cr) catalysts for highly efficient selective catalytic oxidation of NH3","authors":"Lan Hu,&nbsp;Qiuyue Zhao,&nbsp;Xinling Zhang,&nbsp;Huipeng Li,&nbsp;Cheng Bian,&nbsp;Yiqing Zeng","doi":"10.1007/s11164-025-05651-z","DOIUrl":"10.1007/s11164-025-05651-z","url":null,"abstract":"<div><p>Redox sites and acidic sites are the main active sites of bimetallic oxide catalysts used for selective catalytic oxidation of NH<sub>3</sub> (NH<sub>3</sub>-SCO). In this work, three MMoO<i>x</i> (M = Cr, Fe, and Mn) bimetallic oxides catalysts were prepared by simple grinding and calcination to investigate the effect of redox sites (M sites) on the NH<sub>3</sub>-SCO performance. The NH<sub>3</sub>-SCO test results showed that the activity of MMoO<i>x</i> is in the order of CrMoO<i>x</i> &gt; MnMoO<i>x</i> &gt; FeMoO<i>x</i>. The characterization results of H<sub>2</sub>-TPR, O<sub>2</sub>-TPD, NH<sub>3</sub>-TPD, and in situ DRIFTS proposed that the NH<sub>3</sub>-SCO reaction on MMoO<i>x</i> catalysts is proceed via i-SCR mechanism, and the formation of the intermediates of NH<sub>3</sub>-SCR reaction is the decisive reaction step. Owing to the excellent ability in promoting the formation of nitrate/nitrite species, CrMoO<sub><i>x</i></sub> and MnMoO<i>x</i> samples show much higher NH<sub>3</sub>-SCO activity than FeMoO<i>x</i> sample<i>.</i> CrMoO<sub><i>x</i></sub> can facilitate the formation of a large amount of –NH<sub>2</sub> species, which together with nitrate/nitrite species enhance the NH<sub>3</sub>-SCO reaction via i-SCR reaction route. Therefore, CrMoO<sub><i>x</i></sub> shows the highest NH<sub>3</sub>-SCO activity among the MMoO<i>x</i> catalysts. Through this work, the redox sites of bimetallic oxide catalysts are demonstrated as a vital role in inducing the formation of reaction-active intermediates, which highlight the importance of choosing the redox sites in designing NH<sub>3</sub>-SCO catalyst.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4177 - 4190"},"PeriodicalIF":3.5,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145169170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
APTES immobilized copper-doped nitrogen quantum dots (CuNPs@N-GQDs@APTES) nanocatalyst for synthesis of isoxazol-5(4H)-one, dihydropyrano[3,2-c]chromene and dihydropyrano[2,3-c]pyrazoles in aqueous medium APTES固定化铜掺杂氮量子点(CuNPs@N-GQDs@APTES)纳米催化剂在水介质中合成异恶唑-5(4H)- 1,二氢吡喃[3,2-c]铬和二氢吡喃[2,3-c]吡唑
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-26 DOI: 10.1007/s11164-025-05656-8
Kiran Bagade, Arjun Kumbhar
{"title":"APTES immobilized copper-doped nitrogen quantum dots (CuNPs@N-GQDs@APTES) nanocatalyst for synthesis of isoxazol-5(4H)-one, dihydropyrano[3,2-c]chromene and dihydropyrano[2,3-c]pyrazoles in aqueous medium","authors":"Kiran Bagade,&nbsp;Arjun Kumbhar","doi":"10.1007/s11164-025-05656-8","DOIUrl":"10.1007/s11164-025-05656-8","url":null,"abstract":"<div><p>In this report, environmentally benign strategies were developed for one-pot multicomponent synthesis of isoxazol-5(4<i>H</i>)-one, dihydropyrano[3,2-c]chromene and dihydropyrano[2,3-c]pyrazoles in aqueous medium using an efficient, APTES immobilized copper-doped nitrogen quantum dots (CuNPs@N-GQDs@APTES) nanocatalyst. The catalytic superiority of CuNPs@N-GQDs@APTES leads to the synthesis of advanced heterocycles under optimum reaction conditions. The use of green aqueous medium, ambient reaction temperature, short reaction time, and admirable yields (80–96%) are the notable features of these strategies. The catalyst's performance was found superior with respect to time and yield compared to similar reported catalysts. Moreover, the CuNPs@N-GQDs@APTES catalyst exhibited remarkable recyclability over several reaction cycles without significant activity loss.</p><h3>Graphical abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4625 - 4645"},"PeriodicalIF":3.5,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145169167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The effect of hydrochloric acid on photocatalytic hydrogen production of crystalline graphitic carbon nitride 盐酸对结晶氮化石墨碳光催化制氢的影响
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-25 DOI: 10.1007/s11164-025-05657-7
Yang Li
{"title":"The effect of hydrochloric acid on photocatalytic hydrogen production of crystalline graphitic carbon nitride","authors":"Yang Li","doi":"10.1007/s11164-025-05657-7","DOIUrl":"10.1007/s11164-025-05657-7","url":null,"abstract":"<div><p>Crystalline graphitic carbon nitride (CCN) synthesized by molten salt method has been widely used in many fields. However, the CCN prepared by the molten salt method always contains K ions. The influence of these K ions on the photocatalytic performance of CCN is still not clear. In this paper, three kinds of CCN with different structures were prepared by the molten salt method, including heptazine-based crystalline graphitic carbon nitride (HCN), triazine-based graphitic carbon nitride (TCN), and heptazine/triazine-based composite crystalline graphitic carbon nitride (HTCN). The present study elucidates the inhibitory mechanism of unstable potassium ions in carbonized carbon nitride (CCN) on photocatalytic hydrogen evolution through systematic acid treatment experiments. Notably, hydrochloric acid treatment effectively removed excess K<sup>+</sup> ions from HTCN and HCN materials, significantly enhancing their photocatalytic performance. Specifically, the hydrogen evolution rate of HTCN-H (1170.4 μmol h<sup>−1</sup> g<sup>−1</sup>) exhibited a 32.1% increase compared to pristine HTCN (885.9 μmol h<sup>−1</sup> g<sup>−1</sup>). Mechanistic investigations revealed two critical functions of residual K<sup>+</sup> ions: firstly, elevating the valence band position of CCN materials, thereby reducing their redox potential and electron transfer capability; secondly, occupying active catalytic sites that are essential for proton reduction reactions. However, there is no K ion in the structure of TCN, so hydrochloric acid treatment has no significant effect on its photocatalytic activity (from 49.1 to 54.9 μmol h<sup>−1</sup> g<sup>−1</sup>). These findings not only clarify the dual negative effects of alkali metal residues in CCN-based photocatalysts but also provide a strategic approach for optimizing material performance through targeted ion removal.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4519 - 4534"},"PeriodicalIF":3.5,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145169427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Organic-copper coordination drives the formation of Cu(III) intermediates: a novel pathway for peroxymonosulfate activation and quinolone antibiotics degradation 有机铜配位驱动Cu(III)中间体的形成:过氧单硫酸盐活化和喹诺酮类抗生素降解的新途径
IF 3.5 3区 化学
Research on Chemical Intermediates Pub Date : 2025-06-25 DOI: 10.1007/s11164-025-05659-5
Qing Zhao, Lei Zhou, Guangli Xiu
{"title":"Organic-copper coordination drives the formation of Cu(III) intermediates: a novel pathway for peroxymonosulfate activation and quinolone antibiotics degradation","authors":"Qing Zhao,&nbsp;Lei Zhou,&nbsp;Guangli Xiu","doi":"10.1007/s11164-025-05659-5","DOIUrl":"10.1007/s11164-025-05659-5","url":null,"abstract":"<div><p>Copper ions, particularly Cu(II), were generally regarded as poor activators for peroxymonosulfate (PMS) in advanced oxidation processes. However, this study demonstrated that quinolone antibiotics (QNs), a class of widely used antibiotics, can effectively promote PMS in the presence of Cu(II), resulting in the rapid degradation of QNs themselves. High-valent copper species, namely, Cu(III), were identified as the primary reactive intermediates. Mechanistic analysis revealed that enhanced PMS generation Cu(III) formation was highly associated with organic-copper coordination. Notably, the degradation kinetics of 10 different QNs exhibited a strong linear dependence on their coordination constants with Cu(II), quantitatively demonstrating the ligand-specific kinetic enhancement effect. A redox cycle mechanism involving different copper species was proposed, wherein the Cu(II)–QNs complex facilitates electron transfer from PMS to Cu(II), forming monovalent Cu(I), which is subsequently oxidized by PMS through a coupled electron-proton transfer (CEPT) process to generate Cu(III). Results obtained from this study highlight the critical role of contaminant–metal coordination in mediating valence transitions and provide mechanistic insights for optimizing transition metal-catalyzed advanced oxidation processes in water treatment.</p></div>","PeriodicalId":753,"journal":{"name":"Research on Chemical Intermediates","volume":"51 8","pages":"4315 - 4332"},"PeriodicalIF":3.5,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145169428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","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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