Molecular Catalysis最新文献

{"title":"Facile synthesis of Ce-doped WSe2 nanoflowers on Ni foam for improved hydrogen evolution reaction","authors":"Shihuai Zhao ,&nbsp;Huimin Gao ,&nbsp;Yugao Guo ,&nbsp;Qingyin Zhang ,&nbsp;Xiaoming Zhao","doi":"10.1016/j.mcat.2025.115213","DOIUrl":"10.1016/j.mcat.2025.115213","url":null,"abstract":"<div><div>Tungsten selenide (WSe₂) has caused worthwhile concern due to its excellent catalytic properties; it has become an important catalyst in the field of hydrogen precipitation from electrolyzed water. However, tungsten selenide performance remains restricted by insufficient active sites. At present, doping with rare earth elements is an important method to increase the active edge sites and thus significantly improve the electrical conductivity. In this text, we have employed a one-pot solvothermal method to in situ grow Ce-doped WSe₂ nanomaterials on the nickel foam (NF) substrate. The catalytic performance on HER of Ce-WSe₂ was significantly improved due to the appropriate amount of doped Ce. By modifying the morphology and electronic structure of WSe₂, its hydrogen evolution reaction (HER) catalytic activity is further enhanced. In the 1 M KOH solution, 8 %Ce-WSe₂/NF possesses lower overpotentials and Tafel slopes of 82 mV and 88.2 mV dec^‑1 at 10 mA cm^-2, which shows a significant catalytic performance compared with WSe₂. Moreover, the electrocatalyst showed excellent stability with only minor variations over 24 h of continuous catalyst reaction at a current density of 10 mA cm^-2. This job provides a distinct insight into increasing HER active site for WSe₂-based catalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115213"},"PeriodicalIF":3.9,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144178598","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}

{"title":"Room-temperature hydrolysis cleavage of carbon disulfide over a palladium (II)-functionalized Polyarylether","authors":"Xing yu Chen ,&nbsp;Ling Song ,&nbsp;Qing Huang,&nbsp;Xuan-feng Jiang","doi":"10.1016/j.mcat.2025.115240","DOIUrl":"10.1016/j.mcat.2025.115240","url":null,"abstract":"<div><div>The development of low-energy catalysts is crucial for addressing the challenge of removing carbon disulfide contamination. This study presents a Pd(II)-anchored polyarylether where numerous nitrogen atoms coordinate with palladium nitrate. The catalyst demonstrated remarkable activity against carbon disulfide at room temperature. Furthermore, the integration of chemically stable polymers and sacrificial agents enhanced the catalyst's renewability. By synthesizing both experimental and theoretical results, we proposed a reaction pathway whereby hydroxyl nucleophiles attacked the <em>C</em> = <em>S</em> bonds, leading to the formation of carbon dioxide. This research offered significant insights into the pivotal role of immobilized palladium in the hydrolysis of carbon disulfide and underscored the potential of polymers in purifying water from contaminants.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115240"},"PeriodicalIF":3.9,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144178597","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}

{"title":"Embedded nickel-metallofullerenes (Nin@C60) as an effective catalyst for controlled C-C coupling of CO","authors":"Pengfei Liu ,&nbsp;Mingqian Wang ,&nbsp;Wanfei Hu ,&nbsp;Xiaoying Feng ,&nbsp;Xing Gao ,&nbsp;Wei Qian ,&nbsp;Qiang Wang ,&nbsp;Junying Zhang","doi":"10.1016/j.mcat.2025.115242","DOIUrl":"10.1016/j.mcat.2025.115242","url":null,"abstract":"<div><div>The C<img>C coupling of CO plays a crucial role in the reduction of CO/CO₂ to C₂₊ compounds. Controlling the activity and active sites of the catalyst proves to be an effective method to achieve controllable C<img>C coupling. By doping metals into fullerene to form endohedral metallofullerenes (EMF), a strategy emerges to achieve unique catalytic activity. Herein, we report that embedded nickel-metallofullerenes (Ni_n@C₆₀) as an efficient catalyst can achieve controllable C<img>C coupling of CO, thereby promoting the generation of C₂ products. The results show that it is thermodynamically feasible for Ni_n clusters to embed into C₆₀ to form Ni_n@C₆₀, electronic structure analysis reveals that Ni_n clusters can activate C₆₀ through electron transfer. Subsequently, research finds that the physically adsorbed CO on C₆₀ and Ni_n@C₆₀ surface can directly form O*C*CO intermediate through controllable C<img>C coupling, with an extremely low activation energy barrier (0.10 ∼ 0.41 eV). Among them, Ni₆@C₆₀ has the lowest activation energy barrier, which is 0.10 eV. This work provides new theoretical insights into C<img>C controllable coupling and the design of novel catalysts for efficient CO/CO₂ conversion.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115242"},"PeriodicalIF":3.9,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144168499","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}

{"title":"In situ doping derivative construction of MnOx/Mn-ZrO2-C for efficient degradation of NOx","authors":"Qiuju Qin ,&nbsp;Chaolian Zhu ,&nbsp;Donghai Mo ,&nbsp;Zhengjun Chen ,&nbsp;Lihui Dong ,&nbsp;Bin Li ,&nbsp;Liya Zhou","doi":"10.1016/j.mcat.2025.115243","DOIUrl":"10.1016/j.mcat.2025.115243","url":null,"abstract":"<div><div>MnO_x exhibits excellent low temperature activity for degradation NO_x, but its poor SO₂ tolerance restrains its application. Herein, an in situ construction method for MnO_x loading on Mn-doped ZrO₂ carrier with carbon (MnO_x/Mn-ZrO₂-C) derived from Mn(NO₃)₂/UIO-66 by in situ doped pyrolysis–oxidation, in which Mn replaces Zr to modify the electronic structure of the ZrO₂. The MnO_x/Mn-ZrO₂-C with abundant surface oxygen and acid sites showed excellent activity and better SO₂ resistance. A series of characterization results indicated that Mn doping modulates the electron structure of carrier ZrO₂ and enhances the interactions among MnO_x, carbon, and Mn-ZrO₂, resulting in increasing the electron cloud density around Mn and Zr, and consequently, the Mn and Zr on the MnO_x/Mn-ZrO₂-C exhibit poorer sulfiphilic. These findings emphasize the benefits of utilizing a multipronged effect to fabricate highly active and sulfur-resistant NH₃-SCR catalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115243"},"PeriodicalIF":3.9,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144168496","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}

{"title":"Ceria-zirconia supported Pt-Fe bimetallic catalyst for water gas shift reaction with suppressed methanation activity in reformate-simulated gas","authors":"A.M. Gorlova ,&nbsp;A.A. Saraev ,&nbsp;V.N. Rogozhnikov ,&nbsp;P.V. Snytnikov ,&nbsp;D.I. Potemkin","doi":"10.1016/j.mcat.2025.115236","DOIUrl":"10.1016/j.mcat.2025.115236","url":null,"abstract":"<div><div>PtFe/Ce_0.75Zr_0.25O₂ catalysts were prepared using deposition and impregnation techniques and tested in water gas shift reaction in reformate-simulated feed gas. For the catalyst prepared by subsequent deposition of the metals it was observed that iron (mole ratio Pt:Fe ≈ 1.5) provides for inhibition of side reaction of methanation at the temperatures up to 350 °C. The water gas shift reaction rate per Pt surface area was also increased compared to the catalyst without iron (Pt content was the same). XPS analysis of PtFe/Ce_0.75Zr_0.25O₂ showed that there are Pt⁰ and Fe²⁺ cations on the surface in H₂ atmosphere at 150–350 °C. <em>In situ</em> DRIFTS results demonstrated stronger CO adsorption on the Pt-support interfacial sites and higher CO₂ formation rate in the gas phase going from Pt to Pt-Fe system.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115236"},"PeriodicalIF":3.9,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144168498","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}

{"title":"Hydrogenation and Ring-rearrangement of Furfural to Cyclopentanone over Ultralow-loading Ni-Pt Supported on Layered AlOOH","authors":"Yuxuan Wu ,&nbsp;Sen Luan ,&nbsp;Ye Liu ,&nbsp;Tianjiao Wang ,&nbsp;Minghua Dong ,&nbsp;Huizhen Liu ,&nbsp;Buxing Han","doi":"10.1016/j.mcat.2025.115212","DOIUrl":"10.1016/j.mcat.2025.115212","url":null,"abstract":"<div><div>Constructing efficient and inexpensive metal catalysts to produce cyclopentanone (CPO) from furfural (FFL) is of great significance for the utilization of biomass and synthesis of fine chemicals. The synergy of metal site and acid site is a key factor for hydrogenation of carbonyl and ring-rearrangement. Herein, AlOOH is synthesized to support base metal, nickel (1 %), and ultralow-loading platinum (0.1 %) for the complete conversion of CPO from FFL efficiently and selectively, which is difficult to achieve with common Al₂O₃ as support. Through infrared spectroscopy characterization and H₂-temperature-programmed reduction, Ni₁Pt_0.1/AlOOH has stronger adsorption of the hydroxyl group of FFL and tight bonding between metals promotes the reduction of the overall active sites. Comparison to Ni₁/AlOOH and Pt_0.1/AlOOH individually, the addition of 0.1 wt % Pt enables Ni to play the same role as Pt in hydrogenation while being cheaper. Layered AlOOH has higher activity than common Al₂O₃. The structure of layered hydroxides and the use of water as a solvent promote the hydrogenation of aldehyde group and ring-arrangement. Under the optimized conditions (150 °C, 40 bar of H₂, and 6 h), Ni₁Pt_0.1/AlOOH achieves 98 % selectivity for CPO. Isotope labeling experiments revealed that H-H bond cleavage affects both hydrogenation and rearrangement, while O<img>H bond cleavage in water impacts only rearrangement. This study not only developed an ultralow-loading bimetal catalyst for the efficient hydrogenation and ring-rearrangement of FFL to CPO, but also explored the synergy between noble metals and base metals, as well as between metal sites and acid sites.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115212"},"PeriodicalIF":3.9,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144168497","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}

{"title":"Electrodeposition of Bi nanocomposite with MIL-101 derived carbon as gas diffusion layer for CO2 electroreduction with enhanced formate generation","authors":"Xuetong Liu ,&nbsp;Chi Zhang ,&nbsp;Nuoyan Li ,&nbsp;Runfeng Li ,&nbsp;Songlin Lei ,&nbsp;Wei Hong ,&nbsp;Shuguang Deng ,&nbsp;Jun Wang","doi":"10.1016/j.mcat.2025.115235","DOIUrl":"10.1016/j.mcat.2025.115235","url":null,"abstract":"<div><div>Herein, a novel and flexible self-supporting gas diffusion electrode (GDE) was fabricated, which including an electrodeposited Bi nanocomposite as a catalyst layer and MIL-101 derived porous carbon in the gas diffusion layer (GDL). Compared with the conventional fabrication of GDE electrodes, the electrodeposition approach can avoid the tedious drop-casting processes of the catalyst layer (CL). The <em>in situ</em> growth mode by electrodeposition can also ensure the firmly interaction between CL and current collector, thus enhancing the stability of the electrode. Meanwhile, the porous carbon derived from MIL-101 which with a high specific area is conducive for the CO₂ enrichment on the electrode, thus facilitate the reaction with high current density. Owe to the special structure, the resultant catalyst showed excellent performance for electrocatalytic CO₂ reduction reaction (CO₂RR) with enhanced formic acid generation. Notably, at -1.37 V (<em>vs.</em> RHE), a large current density of 400 mA cm^-2 and a high formate Faraday efficiency (FE_formate) of 96.5 % were achieved, and the yield of formic acid reached 46.5 mmol cm^-2 h^-1, which is superior to most electrocatalytic catalysts for CO₂RR. In addition, the FE_formate value remained high (&gt;90 %) over a wide voltage window of 800 mV, and the catalyst also maintained stable operation at industrial current density for 70 h. This work provides a new strategy for the design of GDEs with novel structure to achieve high activity and durability for different electrocatalysis.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115235"},"PeriodicalIF":3.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137849","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}

{"title":"Superhydrophilic/Superaerophobic Ni/NiFe-based electrocatalysts for water electrolysis: A comprehensive review","authors":"Ruirui Zhang ,&nbsp;Yaoxia Yang ,&nbsp;Fuxing Zhou,&nbsp;Bolin Xiong,&nbsp;Zhen Yao,&nbsp;Wei Zeng,&nbsp;Dongfei Sun,&nbsp;Zhiwang Yang,&nbsp;Ziqiang Lei","doi":"10.1016/j.mcat.2025.115234","DOIUrl":"10.1016/j.mcat.2025.115234","url":null,"abstract":"<div><div>Hydrogen production by water electrolysis is a convenient, low-energy and simple process. The generation of hydrogen (H₂) and oxygen (O₂) through water electrolysis is a sustainable option for future clean energy, but it still faces challenges. A large number of gas bubbles are constantly generated during the hydrogen production process. These bubbles easily adhere to the surface of the material and cannot be detached from the surface quickly enough in time. Over time, the accumulation of bubbles relentlessly obscures a large number of otherwise active catalytic sites, severely hindering the mass-transfer process of reactants and products and leading to a dramatic decrease in mass-transfer efficiency. This leads to a significant reduction in the hydrogen production efficiency, which in turn reduces the overall efficiency of water decomposition. Therefore, the design and preparation of electrocatalysts with superhydrophilic/superhydrophobicity is one of the techniques to improve droplet wettability and reduce bubble attachment. Due to the ability of the superhydrophilic droplets to spread and penetrate rapidly on the electrode surface, Moreover, the superhydrophobicity greatly reduces the adhesion of gas bubbles on the electrode surface. As a result, the mass transfer and reaction kinetics involved in the hydrogen exclusion reaction (HER) and oxygen exclusion reaction (OER) were significantly optimized, which in turn enhanced the catalytic process of the oxygen exclusion reaction/hydrogen exclusion reaction. This paper reviews the reaction mechanisms of superhydrophilic/superhydrophobic electrocatalysts, as well as the mechanisms of hydrogen and oxygen precipitation. Special attention is given to various preparation strategies for bimetallic nickel-iron based (NiFe-based) electrocatalysts and the application of heteroatom doping, heterostructures and oxygen vacancies in NiFe-based electrocatalysts. In addition, this review discusses the practical applications of other monometallic, bimetallic, and multimetallic electrocatalysts in the field of efficient electrocatalysis, as well as the challenges and future prospects.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115234"},"PeriodicalIF":3.9,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144123943","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}

{"title":"Challenges and opportunities to design a highly active hydrodesulfurization catalyst: A comprehensive review","authors":"Shalini Arora ,&nbsp;Rupesh Singh ,&nbsp;Rashmi Khan ,&nbsp;Deepak Kunzru ,&nbsp;Sri Sivakumar","doi":"10.1016/j.mcat.2025.115220","DOIUrl":"10.1016/j.mcat.2025.115220","url":null,"abstract":"<div><div>Hydrodesulfurization (HDS) is a catalytic process, which is used in petroleum refineries to reach sulfur levels &lt;5 ppm of energy fuels due to its higher rate and activity for desulfurization. HDS reaction performance is mainly controlled by the sulfided phase of catalysts e.g., NiMoS/CoMoS sites for NiMo/CoMo based catalysts, and the formation of these sites depends on the catalyst design properties such as active metal dispersion, metal-support interaction, physiochemical properties like surface area/porosity and structure/morphology of catalysts based on their preparation methods/sulfidation conditions. In addition, operating conditions of reaction also govern the performance of the HDS process. A significant number of theoretical as well as experimental studies is available in literature, exploring various catalysts/technologies for HDS reaction. This review paper summarizes all these available strategies in detail and specially focuses on the effect of all mentioned parameters on HDS catalyst activity. Further, this work also discusses the required design charactertics for an ideal HDS catalyst. The prime concern of this review study is focused on highlighting and filling the gap between experimental and theoretical explanations for HDS catalysts, which is very important to analyze the HDS process performance.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115220"},"PeriodicalIF":3.9,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144123942","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}

{"title":"Electrochemical C–H silylation of azauracils with hydrosilanes","authors":"Zhihua Zhang ,&nbsp;Jingfang Wang ,&nbsp;Changsheng Qin ,&nbsp;Shuai Zhang ,&nbsp;Yi Sun ,&nbsp;Chenxu Li ,&nbsp;Xinyue Li ,&nbsp;Fanxu Meng ,&nbsp;Fanghua Ji ,&nbsp;Guangbin Jiang","doi":"10.1016/j.mcat.2025.115218","DOIUrl":"10.1016/j.mcat.2025.115218","url":null,"abstract":"<div><div>Polysubstituted azauracils represent highly important nitrogen-containing heterocyclic compounds that are widely found in biologically active molecules. Current synthetic methods primarily rely on expensive transition metals or often toxic photocatalysts to achieve C<img>H functionalization of azauracils, making it imperative to develop simpler and more practical synthetic approaches. Electroorganic synthesis offers an excellent alternative strategy. Herein, we disclose an electrochemical C<img>H silylation method for the synthesis of various silicon-substituted azauracils using azauracils and hydrosilanes as starting materials. This transformation is conducted in an undivided cell, offering operational simplicity, excellent substrate compatibility, and scalability to gram-scale synthesis. Furthermore, this strategy enables the late-stage derivatization of valuable molecules. Mechanistic studies reveal that azauracils capture silicon radicals through three distinct pathways, ultimately generating diverse polysubstituted azauracil derivatives.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"583 ","pages":"Article 115218"},"PeriodicalIF":3.9,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144123941","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}