Chinese Journal of Catalysis最新文献

英文中文

Oxidative steam reforming of HDPE pyrolysis volatiles on Ni catalysts: Effect of the support (Al2O3, ZrO2, SiO2) and promoter (CeO2, La2O3) on the catalyst performance

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60222-6

Mayra Alejandra Suarez , Laura Santamaria , Gartzen Lopez , Enara Fernandez , Martin Olazar , Maider Amutio , Maite Artetxe

High density polyethylene (HDPE) pyrolysis and in-line oxidative steam reforming was carried out in a two-step reaction system consisting of a conical spouted bed reactor and a fluidized bed reactor. Continuous plastic pyrolysis was conducted at 550 °C and the volatiles formed were fed in-line to the oxidative steam reforming step (space-time 3.12 g_cat min g_HDPE⁻¹; ER = 0.2 and steam/plastic = 3) operating at 700 °C. The influence Ni based reforming catalyst support (Al₂O₃, ZrO₂, SiO₂) and promoter (CeO₂, La₂O₃) have on HDPE pyrolysis volatiles conversion and H₂ production was assessed. The catalysts were prepared by the wet impregnation and they were characterized by means of N₂ adsorption-desorption, X-ray fluorescence, temperature-programmed reduction and X-ray powder diffraction. A preliminary study on coke deposition and the deterioration of catalysts properties was carried out, by analyzing the tested catalysts through temperature programmed oxidation of coke, transmission electron microscopy, and N₂ adsorption-desorption. Among the supports tested, ZrO₂ showed the best performance, attaining conversion and H₂ production values of 92.2% and 12.8 wt%, respectively. Concerning promoted catalysts, they led to similar conversion values (around 90%), but significant differences were observed in H₂ production. Thus, higher H₂ productions were obtained on the Ni/La₂O₃-Al₂O₃ catalyst (12.1 wt%) than on CeO₂ promoted catalysts due to La₂O₃ capability for enhancing water adsorption on the catalyst surface.

{"title":"Oxidative steam reforming of HDPE pyrolysis volatiles on Ni catalysts: Effect of the support (Al2O3, ZrO2, SiO2) and promoter (CeO2, La2O3) on the catalyst performance","authors":"Mayra Alejandra Suarez , Laura Santamaria , Gartzen Lopez , Enara Fernandez , Martin Olazar , Maider Amutio , Maite Artetxe","doi":"10.1016/S1872-2067(24)60222-6","DOIUrl":"10.1016/S1872-2067(24)60222-6","url":null,"abstract":"<div><div>High density polyethylene (HDPE) pyrolysis and in-line oxidative steam reforming was carried out in a two-step reaction system consisting of a conical spouted bed reactor and a fluidized bed reactor. Continuous plastic pyrolysis was conducted at 550 °C and the volatiles formed were fed in-line to the oxidative steam reforming step (space-time 3.12 gcat min gHDPE−1; ER = 0.2 and steam/plastic = 3) operating at 700 °C. The influence Ni based reforming catalyst support (Al2O3, ZrO2, SiO2) and promoter (CeO2, La2O3) have on HDPE pyrolysis volatiles conversion and H2 production was assessed. The catalysts were prepared by the wet impregnation and they were characterized by means of N2 adsorption-desorption, X-ray fluorescence, temperature-programmed reduction and X-ray powder diffraction. A preliminary study on coke deposition and the deterioration of catalysts properties was carried out, by analyzing the tested catalysts through temperature programmed oxidation of coke, transmission electron microscopy, and N2 adsorption-desorption. Among the supports tested, ZrO2 showed the best performance, attaining conversion and H2 production values of 92.2% and 12.8 wt%, respectively. Concerning promoted catalysts, they led to similar conversion values (around 90%), but significant differences were observed in H2 production. Thus, higher H2 productions were obtained on the Ni/La2O3-Al2O3 catalyst (12.1 wt%) than on CeO2 promoted catalysts due to La2O3 capability for enhancing water adsorption on the catalyst surface.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 149-162"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Construction of Ni2P/CoP interface for highly efficient electrolysis of urea-assisted hydrogen production at industrial current densities

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60198-1

Borong Lu , Chunmei Lv , Ying Xie , Kai Zhu , Ke Ye , Xiaojin Li

Interface chemical modulation strategies are considered as promising method to prepare electrocatalysts for the urea oxidation reaction (UOR). However, conventional interface catalysts are generally limited by the inherent activity and incompatibility of the individual components themselves, and the irregular charge distribution and slow charge transfer ability between interfaces severely limit the activity of UOR. Therefore, we optimized and designed a Ni₂P/CoP interface with modulated surface charge distribution and directed charge transfer to promote UOR activity. Density functional theorycalculations first predict a regular charge transfer from CoP to Ni₂P, which creates a built-in electric field between Ni₂P and CoP interface. Optimization of the adsorption/desorption process of UOR/HER reaction intermediates leads to the improvement of catalytic activity. Electrochemical impedance spectroscopy and ex situ X-ray photoelectron spectroscopy characterization confirm the unique mechanism of facilitated reaction at the Ni₂P/CoP interface. Electrochemical tests further validated the prediction with excellent UOR/HER activities of 1.28 V and 19.7 mV vs. RHE, at 10 mA cm⁻², respectively. Furthermore, Ni₂P/CoP achieves industrial-grade current densities (500 mA cm⁻²) at 1.75 V and 1.87 V in the overall urea electrolyzer (UOR||HER) and overall human urine electrolyzer (HUOR||HER), respectively, and demonstrates considerable durability.

{"title":"Construction of Ni2P/CoP interface for highly efficient electrolysis of urea-assisted hydrogen production at industrial current densities","authors":"Borong Lu , Chunmei Lv , Ying Xie , Kai Zhu , Ke Ye , Xiaojin Li","doi":"10.1016/S1872-2067(24)60198-1","DOIUrl":"10.1016/S1872-2067(24)60198-1","url":null,"abstract":"<div><div>Interface chemical modulation strategies are considered as promising method to prepare electrocatalysts for the urea oxidation reaction (UOR). However, conventional interface catalysts are generally limited by the inherent activity and incompatibility of the individual components themselves, and the irregular charge distribution and slow charge transfer ability between interfaces severely limit the activity of UOR. Therefore, we optimized and designed a Ni2P/CoP interface with modulated surface charge distribution and directed charge transfer to promote UOR activity. Density functional theorycalculations first predict a regular charge transfer from CoP to Ni2P, which creates a built-in electric field between Ni2P and CoP interface. Optimization of the adsorption/desorption process of UOR/HER reaction intermediates leads to the improvement of catalytic activity. Electrochemical impedance spectroscopy and ex situ X-ray photoelectron spectroscopy characterization confirm the unique mechanism of facilitated reaction at the Ni2P/CoP interface. Electrochemical tests further validated the prediction with excellent UOR/HER activities of 1.28 V and 19.7 mV vs. RHE, at 10 mA cm−2, respectively. Furthermore, Ni2P/CoP achieves industrial-grade current densities (500 mA cm−2) at 1.75 V and 1.87 V in the overall urea electrolyzer (UOR||HER) and overall human urine electrolyzer (HUOR||HER), respectively, and demonstrates considerable durability.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 163-175"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549249","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Surface confinement of sub-1 nm Pt nanoclusters on 1D/2D NiO nanotubes/nanosheets as an effective electrocatalyst for urea-assisted energy-saving hydrogen production

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60203-2

Jiaxin Li , Yan Lv , Xueyan Wu , Xinyu Guo , Zhuojun Yang , Jixi Guo , Tianhua Zhou , Dianzeng Jia

To address the high cost and limited electrochemical endurance of Pt-based electrocatalysts, the appropriate introduction of transition metal-based compounds as supports to disperse and anchor Pt species offers a promising approach for improving catalytic efficiency. In this study, sub-1 nm Pt nanoclusters were uniformly confined on NiO supports with a hierarchical nanotube/nanosheet structure (Pt/NiO/NF) through a combination of spatial domain confinement and annealing. The resulting catalyst exhibited excellent electrocatalytic activity and stability for hydrogen evolution (HER) and urea oxidation reactions (UOR) under alkaline conditions. Structural characterization and density functional theory calculations demonstrated that sub-1 nm Pt nanoclusters were immobilized on the NiO supports by Pt–O–Ni bonds at the interface. The strong metal-support interaction induced massive charge redistribution around the heterointerface, leading to the formation of multiple active sites. The Pt/NiO/NF catalyst only required an overpotential of 12 and 136 mV to actuate current densities of 10 and 100 mA cm⁻² for the HER, respectively, and maintained a voltage retention of 96% for 260 h of continuous operation at a current density of 500 mA cm⁻². Notably, in energy-efficient hydrogen production systems coupled with the HER and UOR, the catalyst required cell voltages of 1.37 and 1.53 V to drive current densities of 10 and 50 mA cm⁻², respectively—approximately 300 mV lower than conventional water electrolysis systems. This study presents a novel pathway for designing highly efficient and robust sub-nanometer metal cluster catalysts.

{"title":"Surface confinement of sub-1 nm Pt nanoclusters on 1D/2D NiO nanotubes/nanosheets as an effective electrocatalyst for urea-assisted energy-saving hydrogen production","authors":"Jiaxin Li , Yan Lv , Xueyan Wu , Xinyu Guo , Zhuojun Yang , Jixi Guo , Tianhua Zhou , Dianzeng Jia","doi":"10.1016/S1872-2067(24)60203-2","DOIUrl":"10.1016/S1872-2067(24)60203-2","url":null,"abstract":"<div><div>To address the high cost and limited electrochemical endurance of Pt-based electrocatalysts, the appropriate introduction of transition metal-based compounds as supports to disperse and anchor Pt species offers a promising approach for improving catalytic efficiency. In this study, sub-1 nm Pt nanoclusters were uniformly confined on NiO supports with a hierarchical nanotube/nanosheet structure (Pt/NiO/NF) through a combination of spatial domain confinement and annealing. The resulting catalyst exhibited excellent electrocatalytic activity and stability for hydrogen evolution (HER) and urea oxidation reactions (UOR) under alkaline conditions. Structural characterization and density functional theory calculations demonstrated that sub-1 nm Pt nanoclusters were immobilized on the NiO supports by Pt–O–Ni bonds at the interface. The strong metal-support interaction induced massive charge redistribution around the heterointerface, leading to the formation of multiple active sites. The Pt/NiO/NF catalyst only required an overpotential of 12 and 136 mV to actuate current densities of 10 and 100 mA cm−2 for the HER, respectively, and maintained a voltage retention of 96% for 260 h of continuous operation at a current density of 500 mA cm−2. Notably, in energy-efficient hydrogen production systems coupled with the HER and UOR, the catalyst required cell voltages of 1.37 and 1.53 V to drive current densities of 10 and 50 mA cm−2, respectively—approximately 300 mV lower than conventional water electrolysis systems. This study presents a novel pathway for designing highly efficient and robust sub-nanometer metal cluster catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 203-218"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Collaborative photocatalytic C–C coupling with Cu and P dual sites to produce C2H4 over CuxP/g-C3N4 heterojunction

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60183-X

Dongxiao Wen , Nan Wang , Jiahe Peng , Tetsuro Majima , Jizhou Jiang

Light-driven CO₂ reduction reaction (CO₂RR) to value-added ethylene (C₂H₄) holds significant promise for addressing energy and environmental challenges. While the high energy barriers for *CO intermediates hydrogenation and C–C coupling limit the C₂H₄ generation. Herein, Cu_xP/g-C₃N₄ heterojunction prepared by an in-situ phosphating technique, achieved collaborative photocatalytic CO₂ and H₂O, producing CO and C₂H₄ as the main products. Notably, the selectivity of C₂H₄ produced by Cu_xP/g-C₃N₄ attained to 64.25%, which was 9.85 times that of Cu_xP (6.52%). Detailed time-resolution photoluminescence spectra, femtosecond transient absorption spectroscopy tests and density functional theory (DFT) calculation validate the ultra-fast interfacial electron transfer mechanism in Cu_xP/g-C₃N₄ heterojunction. Successive *H on P sites caused by adsorbed H₂O splitting with moderate hydrogenation ability enables the multi-step hydrogenation during CO₂RR process over Cu_xP/g-C₃N₄. With the aid of mediated asymmetric Cu and P dual sites by g-C₃N₄ nanosheet, the produced *CHO shows an energetically favorable for C–C coupling. The coupling formed *CHOCHO further accepts photoexcited efficient e^– and *H to deeply produce C₂H₄ according to the C2+ intermediates, which has been detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and interpreted by DFT calculation. The novel insight mechanism offers an essential understanding for the development of Cu_xP-based heterojunctions for photocatalytic CO₂ to C2+ value-added fuels.

{"title":"Collaborative photocatalytic C–C coupling with Cu and P dual sites to produce C2H4 over CuxP/g-C3N4 heterojunction","authors":"Dongxiao Wen , Nan Wang , Jiahe Peng , Tetsuro Majima , Jizhou Jiang","doi":"10.1016/S1872-2067(24)60183-X","DOIUrl":"10.1016/S1872-2067(24)60183-X","url":null,"abstract":"<div><div>Light-driven CO2 reduction reaction (CO2RR) to value-added ethylene (C2H4) holds significant promise for addressing energy and environmental challenges. While the high energy barriers for *CO intermediates hydrogenation and C–C coupling limit the C2H4 generation. Herein, CuxP/g-C3N4 heterojunction prepared by an in-situ phosphating technique, achieved collaborative photocatalytic CO2 and H2O, producing CO and C2H4 as the main products. Notably, the selectivity of C2H4 produced by CuxP/g-C3N4 attained to 64.25%, which was 9.85 times that of CuxP (6.52%). Detailed time-resolution photoluminescence spectra, femtosecond transient absorption spectroscopy tests and density functional theory (DFT) calculation validate the ultra-fast interfacial electron transfer mechanism in CuxP/g-C3N4 heterojunction. Successive *H on P sites caused by adsorbed H2O splitting with moderate hydrogenation ability enables the multi-step hydrogenation during CO2RR process over CuxP/g-C3N4. With the aid of mediated asymmetric Cu and P dual sites by g-C3N4 nanosheet, the produced *CHO shows an energetically favorable for C–C coupling. The coupling formed *CHOCHO further accepts photoexcited efficient e– and *H to deeply produce C2H4 according to the C2+ intermediates, which has been detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and interpreted by DFT calculation. The novel insight mechanism offers an essential understanding for the development of CuxP-based heterojunctions for photocatalytic CO2 to C2+ value-added fuels.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 58-74"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Modular three-component radical fluoroalkyl-sulfuration of unactivated alkenes

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60190-7

Gao-feng Yang , Zhi Liu , Kai Liu , Xiaopeng Wu , Chengjian Zhu , Weipeng Li , Jin Xie

The accompanied forge of C(sp³)–S and C(sp³)–C(sp³) bonds across alkene frameworks serves as a potent strategy to construct biologically important compounds. Here, we report a metal-free, photochemically mediated fluoroalkyl-mono/disulfuration of unactivated alkenes with high efficiency and high selectivity. A wide range of terminal and internal alkenes are good coupling partners, affording the expected products in moderate to good yields (>90 examples). The exceedingly mild reaction conditions, exceptional functional group tolerance, broad substrate scope, and the potential for late-stage modifications of pharmaceutical molecules highlight the utility of this method in the preparation of privileged motifs from readily available disulfides, tetrasulfides, and diselenides. Mechanistic studies suggest that a secondary alkyl radical intermediate undergoes efficient homolytic substitution with disulfides, facilitating the modular synthesis of a diverse array of unsymmetrical thioethers.

{"title":"Modular three-component radical fluoroalkyl-sulfuration of unactivated alkenes","authors":"Gao-feng Yang , Zhi Liu , Kai Liu , Xiaopeng Wu , Chengjian Zhu , Weipeng Li , Jin Xie","doi":"10.1016/S1872-2067(24)60190-7","DOIUrl":"10.1016/S1872-2067(24)60190-7","url":null,"abstract":"<div><div>The accompanied forge of C(sp3)–S and C(sp3)–C(sp3) bonds across alkene frameworks serves as a potent strategy to construct biologically important compounds. Here, we report a metal-free, photochemically mediated fluoroalkyl-mono/disulfuration of unactivated alkenes with high efficiency and high selectivity. A wide range of terminal and internal alkenes are good coupling partners, affording the expected products in moderate to good yields (>90 examples). The exceedingly mild reaction conditions, exceptional functional group tolerance, broad substrate scope, and the potential for late-stage modifications of pharmaceutical molecules highlight the utility of this method in the preparation of privileged motifs from readily available disulfides, tetrasulfides, and diselenides. Mechanistic studies suggest that a secondary alkyl radical intermediate undergoes efficient homolytic substitution with disulfides, facilitating the modular synthesis of a diverse array of unsymmetrical thioethers.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 249-258"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549187","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Cation and anion modulation activates lattice oxygen for enhanced oxygen evolution

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60176-2

Mingxing Chen , Zihe Du , Nian Liu , Huijie Li , Jing Qi , Enbo Shangguan , Jing Li , Jiahao Cao , Shujiao Yang , Wei Zhang , Rui Cao

Oxygen evolution reaction (OER) is often regarded as a crucial bottleneck in the field of renewable energy storage and conversion. To further accelerate the sluggish kinetics of OER, a cation and anion modulation strategy is reported here, which has been proven to be effective in preparing highly active electrocatalyst. For example, the cobalt, sulfur, and phosphorus modulated nickel hydroxide (denoted as NiCoPSOH) only needs an overpotential of 232 mV to reach a current density of 20 mA cm^–2, demonstrating excellent OER performances. The cation and anion modulation facilitates the generation of high-valent Ni species, which would activate the lattice oxygen and switch the OER reaction pathway from conventional adsorbate evolution mechanism to lattice oxygen mechanism (LOM), as evidenced by the results of electrochemical measurements, Raman spectroscopy and differential electrochemical mass spectrometry. The LOM pathway of NiCoPSOH is further verified by the theoretical calculations, including the upshift of O 2p band center, the weakened Ni–O bond and the lowest energy barrier of rate-limiting step. Thus, the anion and cation modulated catalyst NiCoPSOH could effectively accelerate the sluggish OER kinetics. Our work provides a new insight into the cation and anion modulation, and broadens the possibility for the rational design of highly active electrocatalysts.

{"title":"Cation and anion modulation activates lattice oxygen for enhanced oxygen evolution","authors":"Mingxing Chen , Zihe Du , Nian Liu , Huijie Li , Jing Qi , Enbo Shangguan , Jing Li , Jiahao Cao , Shujiao Yang , Wei Zhang , Rui Cao","doi":"10.1016/S1872-2067(24)60176-2","DOIUrl":"10.1016/S1872-2067(24)60176-2","url":null,"abstract":"<div><div>Oxygen evolution reaction (OER) is often regarded as a crucial bottleneck in the field of renewable energy storage and conversion. To further accelerate the sluggish kinetics of OER, a cation and anion modulation strategy is reported here, which has been proven to be effective in preparing highly active electrocatalyst. For example, the cobalt, sulfur, and phosphorus modulated nickel hydroxide (denoted as NiCoPSOH) only needs an overpotential of 232 mV to reach a current density of 20 mA cm–2, demonstrating excellent OER performances. The cation and anion modulation facilitates the generation of high-valent Ni species, which would activate the lattice oxygen and switch the OER reaction pathway from conventional adsorbate evolution mechanism to lattice oxygen mechanism (LOM), as evidenced by the results of electrochemical measurements, Raman spectroscopy and differential electrochemical mass spectrometry. The LOM pathway of NiCoPSOH is further verified by the theoretical calculations, including the upshift of O 2p band center, the weakened Ni–O bond and the lowest energy barrier of rate-limiting step. Thus, the anion and cation modulated catalyst NiCoPSOH could effectively accelerate the sluggish OER kinetics. Our work provides a new insight into the cation and anion modulation, and broadens the possibility for the rational design of highly active electrocatalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 282-291"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Boosting H2O2 evolution of CdS via constructing a ternary photocatalyst with earth-abundant halloysite nanotubes and NiS co-catalyst

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-02-01 DOI: 10.1016/S1872-2067(24)60191-9

Hongfen Li , Yihe Zhang , Jianming Li , Qing Liu , Xiaojun Zhang , Youpeng Zhang , Hongwei Huang

Hydrogen peroxide (H₂O₂), an environmentally friendly chemical with high value, is extensively used in industrial production and daily life. However, the traditional anthraquinone method for H₂O₂ production is associated with a highly energy-consuming and heavily polluting process. Solor-driven photocatalytic evolution of H₂O₂ is a promising, eco-friendly, and energy-efficient strategy that holds great potential to substitute the traditional approach. Here, a ternary photocatalyst, NiS/CdS/Halloysite nanotubes (NiS/CdS/HNTs) is designed and prepared with an earth-abundant clay mineral HNTs as the support and NiS as a co-catalyst. The pivotal roles of HNTs and NiS in the photocatalytic process are elucidated by experiments and theoretical calculations. HNTs serve as the carrier, which allows CdS to be uniformly dispersed onto its surface as small particles, increasing effective contact with H₂O and O₂ for H₂O₂ formation. Simultaneously, it resulted in the formation of a Schottky junction between NiS and CdS, which not only favors photogenerated charges separating efficiently but also provides a unidirectional path to transfer electrons. Consequently, the optimized NiS/CdS/HNTs composite demonstrates an H₂O₂ evolution rate of 380.5 μmol·g⁻¹·h⁻¹ without adding any sacrificial agent or extra O₂, nearly 5.0 times that of pure CdS. This work suggests a feasible idea for designing and developing highly active and low-cost solar energy catalytic composite materials.

{"title":"Boosting H2O2 evolution of CdS via constructing a ternary photocatalyst with earth-abundant halloysite nanotubes and NiS co-catalyst","authors":"Hongfen Li , Yihe Zhang , Jianming Li , Qing Liu , Xiaojun Zhang , Youpeng Zhang , Hongwei Huang","doi":"10.1016/S1872-2067(24)60191-9","DOIUrl":"10.1016/S1872-2067(24)60191-9","url":null,"abstract":"<div><div>Hydrogen peroxide (H2O2), an environmentally friendly chemical with high value, is extensively used in industrial production and daily life. However, the traditional anthraquinone method for H2O2 production is associated with a highly energy-consuming and heavily polluting process. Solor-driven photocatalytic evolution of H2O2 is a promising, eco-friendly, and energy-efficient strategy that holds great potential to substitute the traditional approach. Here, a ternary photocatalyst, NiS/CdS/Halloysite nanotubes (NiS/CdS/HNTs) is designed and prepared with an earth-abundant clay mineral HNTs as the support and NiS as a co-catalyst. The pivotal roles of HNTs and NiS in the photocatalytic process are elucidated by experiments and theoretical calculations. HNTs serve as the carrier, which allows CdS to be uniformly dispersed onto its surface as small particles, increasing effective contact with H2O and O2 for H2O2 formation. Simultaneously, it resulted in the formation of a Schottky junction between NiS and CdS, which not only favors photogenerated charges separating efficiently but also provides a unidirectional path to transfer electrons. Consequently, the optimized NiS/CdS/HNTs composite demonstrates an H2O2 evolution rate of 380.5 μmol·g−1·h−1 without adding any sacrificial agent or extra O2, nearly 5.0 times that of pure CdS. This work suggests a feasible idea for designing and developing highly active and low-cost solar energy catalytic composite materials.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 111-122"},"PeriodicalIF":15.7,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143549193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Metal species confined in metal-organic frameworks for CO2 hydrogenation: Synthesis, catalytic mechanisms, and future perspectives

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-01-01 DOI: 10.1016/S1872-2067(24)60177-4

Bailing Zhong , Jundie Hu , Xiaogang Yang , Yinying Shu , Yahui Cai , Chang Ming Li , Jiafu Qu

ABSTRACT

Metal-organic frameworks (MOFs) serve as highly effective hosts for ultrasmall metal species, creating advanced nanocatalysts with superior catalytic performance, stability, and selective activity. The synergistic interplay between metal species confined within MOF nanopores and their active sites enhances catalytic efficiency in CO₂ hydrogenation reactions. Herein, recent advancements in synthesizing metal-confined MOFs are discussed, along with their applications in catalyzing CO₂ conversion through various methods such as photocatalysis, thermal catalysis, and photothermal catalysis. Additionally, we further emphasize the fundamental principles and factors that influence various types of catalytic CO₂ hydrogenation reactions, while offering insights into future research directions in this dynamic field.

引用次数: 0

Electrochemical CO2RR to C2+ products: A vision of dynamic surfaces of Cu-based catalysts

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-01-01 DOI: 10.1016/S1872-2067(24)60185-3

Jinxin Wang, Jiaqi Zhang, Chen Chen

ABSTRACT

Electrochemical reduction of CO₂ (CO₂RR) to form high-energy-density and high-value-added multicarbon products has attracted much attention. Selective reduction of CO₂ to C₂₊ products face the problems of low reaction rate, complex mechanism and low selectivity. Currently, except for a few examples, copper-based catalysts are the only option capable of achieving efficient generation of C₂₊ products. However, the continuous dynamic reconstruction of the catalyst causes great difficulty in understanding the structure-performance relationship of CO₂RR. In this review, we first discuss the mechanism of C₂₊ product generation. The structural factors promoting C₂₊ product generation are outlined, and the dynamic evolution of these structural factors is discussed. Furthermore, the effects of electrolyte and electrolysis conditions are reviewed in a vision of dynamic surface. Finally, further exploration of the reconstruction mechanism of Cu-based catalysts and the application of emerging robotic AI chemists are discussed.

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引用次数: 0

Revisiting the origin of the superior performance of defective zirconium oxide catalysts in propane dehydrogenation: Double-edged oxygen vacancy

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2025-01-01 DOI: 10.1016/S1872-2067(24)60163-4

Yuqing Tang , Yanjun Chen , Aqsa Abid , Zichun Meng , Xiaoying Sun , Bo Li , Zhen Zhao

ABSTRACT

Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation, which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites (Zr_cus) around the oxygen vacancies. The origin of the enhanced catalytic activity of ZrO₂ with defective tetrahedral Zr sites was examined by direct comparison with its pristine counterpart in the current study. Electronic-structure analysis revealed that electrons from oxygen removal were localized within vacancies on the defective surface, which directly attacked the C–H bond in propane. The involvement of localized electrons activates the C–H bond via back-donation to the antibonding orbital on the defective surface; conversely, charge is transferred from propane to the pristine surfaces. The barrier for the first C–H bond activation is clearly significantly reduced on the defective surfaces compared to that on the pristine surfaces, which verifies the superior activity of Zr_cus. Notably, however, the desorption of both propene and hydrogen molecules from Zr_cus is more difficult due to strong binding. The calculated turnover frequency (TOF) for propene formation demonstrates that the pristine surfaces exhibit better catalytic performance at lower temperatures, whereas the defective surfaces have a larger TOF at high temperatures. However, the rate-determining step and reaction order on the defective surface differ from those on the pristine surface, which corroborates that the catalysts follow different mechanisms. A further optimization strategy was proposed to address the remaining bottlenecks in propane dehydrogenation on zirconium oxide.

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引用次数: 0

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