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学者姓名：卢雪峰
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Abstract ：
The artificial disturbance in the nitrogen cycle has necessitated an urgent need for nitric oxide (NO) removal. Electrochemical technologies for NO conversion have gained increasing attention in recent years. This comprehensive review presents the recent advancements in selective electrocatalytic conversion of NO to high value-added chemicals, with specific emphasis on catalyst design, electrolyte composition, mass diffusion, and adsorption energies of key intermediate species. Furthermore, the review explores the synergistic electrochemical co-electrolysis of NO with specific carbon source molecules, enabling the synthesis of a range of valuable chemicals with CN bonds. It also provides in-depth insights into the intricate reaction pathways and underlying mechanisms, offering valuable perspectives on the challenges and prospects of selective NO electrolysis. By advancing comprehension and fostering awareness of nitrogen cycle balance, this review contributes to the development of efficient and sustainable electrocatalytic systems for the selective synthesis of valuable chemicals from NO. The artificially induced imbalance in the nitrogen cycle necessitates urgent need for NO removal. This review highlights recent advances in selective electrocatalytic NO conversion into valuable chemicals, emphasizing catalyst design, electrolyte composition, mass diffusion, and adsorption energies. It elucidates reaction pathways and mechanisms, providing insights into the challenges and prospects of NO electrolysis and enhancing awareness of the nitrogen cycle. image
Keyword ：
CN bond CN bond electrocatalysis electrocatalysis electrolyte electrolyte NO oxidation NO oxidation NO reduction NO reduction
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| GB/T 7714 | Wang, Dongdong , Lu, Xue Feng , Luan, Deyan et al. Selective Electrocatalytic Conversion of Nitric Oxide to High Value-Added Chemicals [J]. | ADVANCED MATERIALS , 2024 , 36 (18) . |
| MLA | Wang, Dongdong et al. "Selective Electrocatalytic Conversion of Nitric Oxide to High Value-Added Chemicals" . | ADVANCED MATERIALS 36 . 18 (2024) . |
| APA | Wang, Dongdong , Lu, Xue Feng , Luan, Deyan , Lou, Xiong Wen (David) . Selective Electrocatalytic Conversion of Nitric Oxide to High Value-Added Chemicals . | ADVANCED MATERIALS , 2024 , 36 (18) . |
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The selective conversion of ethane (C2H6) to ethylene (C2H4) under mild conditions is highly wanted, yet very challenging. Herein, it is demonstrated that a Pt/WO3-x catalyst, constructed by supporting ultrafine Pt nanoparticles on the surface of oxygen-deficient tungsten oxide (WO3-x) nanoplates, is efficient and reusable for photocatalytic C2H6 dehydrogenation to produce C2H4 with high selectivity. Specifically, under pure light irradiation, the optimized Pt/WO3-x photocatalyst exhibits C2H4 and H2 yield rates of 291.8 and 373.4 mu mol g-1 h-1, respectively, coupled with a small formation of CO (85.2 mu mol g-1 h-1) and CH4 (19.0 mu mol g-1 h-1), corresponding to a high C2H4 selectivity of 84.9%. Experimental and theoretical studies reveal that the vacancy-rich WO3-x catalyst enables broad optical harvesting to generate charge carriers by light for working the redox reactions. Meanwhile, the Pt cocatalyst reinforces adsorption of C2H6, desorption of key reaction species, and separation and migration of light-induced charges to promote the dehydrogenation reaction with high productivity and selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculation expose the key intermediates formed on the Pt/WO3-x catalyst during the reaction, which permits the construction of the possible C2H6 dehydrogenation mechanism. The Pt/WO3-x photocatalyst consisted of ultrafine Pt nanoparticles supported on the surface of oxygen-defective tungsten oxide nanoplates manifests high activity and fine reusability for selective ethylene formation from ethane dehydrogenation by simulated sunlight under mild conditions. image
Keyword ：
ethylene production ethylene production lattice oxygen lattice oxygen oxygen vacancy oxygen vacancy photocatalysis photocatalysis tungsten oxide tungsten oxide
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| GB/T 7714 | Liu, Yue , Xue, Weichao , Liu, Xiaoqing et al. Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis [J]. | SMALL , 2024 . |
| MLA | Liu, Yue et al. "Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis" . | SMALL (2024) . |
| APA | Liu, Yue , Xue, Weichao , Liu, Xiaoqing , Wei, Fen , Lin, Xiahui , Lu, Xue Feng et al. Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis . | SMALL , 2024 . |
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Aerobic photocatalytic oxidation is considered as an efficient and green method to remedy low-concentration H2S pollutants associated with the energy and chemical industries. However, the fabrication of a sulfur-resistant catalyst with good performance is a great challenge because of the poisoning effect of H2S and the difficulty in oxygen (O-2) activation. Herein, a photocatalytic hybrid material composed of chemically stable cobalt phosphide (CoP) and structural base-enriched carbon nitride (CN) was developed for the efficient oxidation of H2S, which could achieve 95% H2S conversion, and its service time could last more than 35 h with over 80% H2S conversion. Reflecting from the characterizations and theoretical simulations, the enhanced H2S conversion was on account that CoP could stimulate the electrons shuttling from the photocatalytic system towards the gaseous O-2, facilitating the production of critical superoxide radical via the O-2 reduction process and accelerating the surface H2S oxidation process. This work provides new insights into the design of a sustainable photocatalytic oxidation system for the treatment of chemically active contaminants through constructing stable interfacial electron transfer channels for prominent O-2 activation.
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| GB/T 7714 | Wang, Jiali , Chen, Biqi , Zeng, Fanghua et al. Boosting oxygen activation by CoP/carbon nitride photocatalyst in low-concentration H2S oxidation [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 . |
| MLA | Wang, Jiali et al. "Boosting oxygen activation by CoP/carbon nitride photocatalyst in low-concentration H2S oxidation" . | JOURNAL OF MATERIALS CHEMISTRY A (2024) . |
| APA | Wang, Jiali , Chen, Biqi , Zeng, Fanghua , Lu, Xue Feng , Hou, Yidong , Lin, Wei et al. Boosting oxygen activation by CoP/carbon nitride photocatalyst in low-concentration H2S oxidation . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 . |
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Thermal catalytic oxidative dehydrogenation of ethane with O2 has been extensively studied as an approach for ethene production, but this approach is energy intensive and has disadvantages of overoxidation, high-cost and safety concerns. Herein, we present ZnO-supported Pt nanoparticles that are highly active and selective for dehydrogenating ethane to ethene with simulated sunlight via a photo-supported Mars-van Krevelen mechanism. The Pt/ZnO catalyst achieves a high ethane-to-ethene conversion rate of 867.8 mu mol h-1 g-1 and an excellent selectivity of 97.56%. Besides, it is also coking-resistant and can be readily revived by exposure to O2 for refilling the consumed lattice oxygen to preserve its original activity. It is revealed that the Pt species facilitate C2H4 desorption from the catalyst to inhibit overoxidation and enhance separation of light-induced charges to boost the photocatalytic efficiency. Whilst the photogenerated holes on ZnO are captured by surface lattice oxygen to generate active O- species, H atoms were extracted from adsorbed C2H6 to produce C2H4. In situ diffuse reflectance infrared Fourier transform spectroscopy is applied to detect the key intermediates and thus propose the possible catalytic EDH process over the Pt/ZnO photocatalyst. A Pt/ZnO photocatalyst is efficient and reusable for ethene production from ethane dehydrogenation with simulated sunlight, affording outstanding C2H4 productivity of 867.8 mu mol h-1 g-1 and selectivity of 97.56%.
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| GB/T 7714 | Guo, Wenyu , Shi, Wenwen , Cai, Junjian et al. Photocatalytic ethene synthesis from ethane dehydrogenation with high selectivity by ZnO-supported Pt nanoparticles [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2024 . |
| MLA | Guo, Wenyu et al. "Photocatalytic ethene synthesis from ethane dehydrogenation with high selectivity by ZnO-supported Pt nanoparticles" . | CATALYSIS SCIENCE & TECHNOLOGY (2024) . |
| APA | Guo, Wenyu , Shi, Wenwen , Cai, Junjian , Wei, Fen , Lin, Xiahui , Lu, Xuefeng et al. Photocatalytic ethene synthesis from ethane dehydrogenation with high selectivity by ZnO-supported Pt nanoparticles . | CATALYSIS SCIENCE & TECHNOLOGY , 2024 . |
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The photocatalytic selective oxidation of CH4 to value-added higher hydrocarbons presents a promising avenue for the sustainable development of the chemical industry; however, the mild activation and conversion of CH4 remain great challenges. Herein, a novel Au/Zn2Ti3O8 hybrid photocatalyst is assembled from supporting Au nanoparticles (NPs) on the surface of Zn2Ti3O8 nanospheres. The Zn2Ti3O8 semiconductor with Zn2+ active sites drives the CH4 coupling reaction, while the Au NPs promote the separation and migration of charge carriers. When irradiated with a 365 LED light, the 1.0%-Au/Zn2Ti3O8 catalyst exhibits high activity and stability for selective CH4 coupling with O2, affording an optimal C2H6 yield of 609.49 μmol g−1 h−1 with 80.18% selectivity, which is among the state-of-the-art values under comparable conditions. Besides, the 1.0%-Au/Zn2Ti3O8 sample affords a turnover number (TON) of 239.1 and an apparent quantum efficiency (AQE) of 1.05% at 365 nm. Studies reveal that the Schottky junction interface strongly promotes photoinduced electrons to be transferred to Au from Zn2Ti3O8, realizing directed separation and migration of charge carriers for high photocatalytic activity. Various in situ spectroscopy analyses expose that the key ˙CH3 species in CH4-to-C2H6 conversion are stabilized by the surface Au sites for the subsequent coupling reaction to form C2H6, which prevents the undesirable overoxidation reaction to afford high C2H6 selectivity. A possible photocatalytic oxidative CH4 coupling mechanism over the Au/Zn2Ti3O8 hybrid is also proposed. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Huang, Q. , Cai, J. , Wei, F. et al. Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions [J]. | Journal of Materials Chemistry A , 2024 , 12 (32) : 21334-21340 . |
| MLA | Huang, Q. et al. "Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions" . | Journal of Materials Chemistry A 12 . 32 (2024) : 21334-21340 . |
| APA | Huang, Q. , Cai, J. , Wei, F. , Fan, Y. , Liang, Z. , Liu, K. et al. Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions . | Journal of Materials Chemistry A , 2024 , 12 (32) , 21334-21340 . |
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Rare-earth (RE)-based materials are evolving as a promising paradigm for the electrocatalytic oxygen reduction reaction (ORR) to lead the practical application in energy conversion technologies. However, the systematic comprehension of the catalytic role of RE in the enhanced ORR is still limited. Herein, we develop a novel RE-based catalyst consisting of atomic Co species coupled with Tb2O3 (Co@Tb2O3) to unveil the role of RE in enhanced ORR performance. Co@Tb2O3 delivers satisfactory ORR activity with an onset potential and half-wave potential of 1.02 VRHE and 0.85 VRHE, respectively, outperforming the Pt/C benchmark and many reported Co-based catalysts. Quasi-operando X-ray photoemission spectroscopy exhibits potential-dependent shifts of binding energy and full width at half maximum for Co 2p and Tb 3d/4d, demonstrating the successful coverage and transformation of oxygen intermediates during the ORR. Theoretical calculations uncover that the constructed [Co-O-Tb] unit site in Co@Tb2O3 endows Co 3d with a narrow band and appropriate band location via the gradient orbital coupling of Co 3d-O 2p-Tb 4f. Such narrow-band behavior in the [Co-O-Tb] unit site makes the interaction between the Co site and oxygen intermediates in the form of an ideal sigma/pi bond mixing type, which provides flexible binding strength of oxygen intermediates, thus breaking the scaling relation of *OOH and*OH to be closer to optimal conditions. We believe that this work would set a new understanding for the design of high-efficiency RE-based materials towards the ORR. Tb2O3 endows Co 3d with a narrow band and appropriate band location via Co 3d-O 2p-Tb 4f gradient orbital coupling to efficiently enhance the oxygen reduction reaction.
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| GB/T 7714 | Wang, Xuan , Zhang, Juan , Wang, Pu et al. Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2023 , 16 (11) : 5500-5512 . |
| MLA | Wang, Xuan et al. "Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction" . | ENERGY & ENVIRONMENTAL SCIENCE 16 . 11 (2023) : 5500-5512 . |
| APA | Wang, Xuan , Zhang, Juan , Wang, Pu , Li, Liangcheng , Wang, Huiyu , Sun, Dongmei et al. Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction . | ENERGY & ENVIRONMENTAL SCIENCE , 2023 , 16 (11) , 5500-5512 . |
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Thermocatalytic nonoxidative ethane dehydrogenation (EDH) is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability; exploring technology that permits efficient EDH by solar energy remains a giant challenge. Herein, we present that an oxygen vacancy (Ov)-rich LaVO4 (LaVO4-Ov) catalyst is highly active and stable for photocatalytic EDH, through a dynamic lattice oxygen (Olatt.) and Ov co-mediated mechanism. Irradiated by simulated sunlight at mild conditions, LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a conversion of 2.3%. By loading a small amount of Pt cocatalyst, the evolution and selectivity of C2H4 are enhanced to 275 mu mol h-1 g-1 and 96.8%. Of note, LaVO4-Ov appears nearly no carbon deposition after the reaction. The isotope tracked reactions reveal that the consumed Olatt. recuperates by exposing the used catalyst with O2, thus establishing a dynamic cycle of Olatt. and achieving a facile catalyst regeneration to preserve its intrinsic activity. The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305. The Ov promotes photo absorption, boosts ethane adsorption/activation, and accelerates charge separation/transfer, thus improving the photocatalytic efficiency. The possible photocatalytic EDH mechanism is proposed, considering the key intermediates predicted by density functional theory (DFT) and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS).(c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword ：
Ethane dehydrogenation Ethane dehydrogenation Ethene Ethene LaVO4 LaVO4 Oxygen vacancy Oxygen vacancy Photocatalysis Photocatalysis
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| GB/T 7714 | Wei, Fen , Xue, Weichao , Yu, Zhiyang et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst [J]. | CHINESE CHEMICAL LETTERS , 2023 , 35 (3) . |
| MLA | Wei, Fen et al. "Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst" . | CHINESE CHEMICAL LETTERS 35 . 3 (2023) . |
| APA | Wei, Fen , Xue, Weichao , Yu, Zhiyang , Lu, Xue Feng , Wang, Sibo , Lin, Wei et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst . | CHINESE CHEMICAL LETTERS , 2023 , 35 (3) . |
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Hydrogen is praised as a promising carrier of clean energy due to its high calorific combustion value and environmental friendliness. The idea of water electrolysis powered by renewable electricity to produce high-quality hydrogen has ignited fervor among researchers in pursuit of sustainable energy development. However, the sluggish kinetics of the traditional anodic oxygen evolution reaction (OER) hinders efficient energy conversion. Given this, researchers propose new ideas to improve energy conversion efficiency by developing alternative anodic reaction types and catalysts. This review focuses on nickel-based electrocatalysts, highlighting their recent advancements in conventional OER as well as emerging small molecule electrooxidation reactions. We provide insights into catalyst design and synthesis, performance optimization, mechanism exploration, and structure-activity relationships. Additionally, we discuss the current challenges and potential solutions of Ni-based anode electrocatalysts for hydrogen production.
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| GB/T 7714 | Liu, Jiaqing , Du, Yubei , Zheng, Dandan et al. Nickel-Based Anode Electrocatalysts for Hydrogen Production [J]. | ACS MATERIALS LETTERS , 2023 , 6 (2) : 466-481 . |
| MLA | Liu, Jiaqing et al. "Nickel-Based Anode Electrocatalysts for Hydrogen Production" . | ACS MATERIALS LETTERS 6 . 2 (2023) : 466-481 . |
| APA | Liu, Jiaqing , Du, Yubei , Zheng, Dandan , Wang, Sibo , Hou, Yidong , Zhang, Jiujun et al. Nickel-Based Anode Electrocatalysts for Hydrogen Production . | ACS MATERIALS LETTERS , 2023 , 6 (2) , 466-481 . |
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Manipulating the intrinsic activity of heterogeneous catalysts at the atomic level is an effective strategy to improve the electrocatalytic performances but remains challenging. Here, atomically dispersed Ni anchored on CeO2 particles entrenched on peanut-shaped hollow nitrogen-doped carbon structures (a-Ni/CeO2@NC) is rationally designed and synthesized. The as-prepared a-Ni/CeO2@NC catalyst exhibits substantially boosted intrinsic activity and greatly reduced overpotential for the electrocatalytic oxygen evolution reaction. Experimental and theoretical results demonstrate that the decoration of isolated Ni species over the CeO2 induces electronic coupling and redistribution, thus resulting in the activation of the adjacent Ce sites around Ni atoms and greatly accelerated oxygen evolution kinetics. This work provides a promising strategy to explore the electronic regulation and intrinsic activity improvement at the atomic level, thereby improving the electrocatalytic activity.
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| GB/T 7714 | Pei, Zhihao , Zhang, Huabin , Wu, Zhi-Peng et al. Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity [J]. | SCIENCE ADVANCES , 2023 , 9 (26) . |
| MLA | Pei, Zhihao et al. "Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity" . | SCIENCE ADVANCES 9 . 26 (2023) . |
| APA | Pei, Zhihao , Zhang, Huabin , Wu, Zhi-Peng , Lu, Xue Feng , Luan, Deyan , Lou, Xiong Wen (David) . Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity . | SCIENCE ADVANCES , 2023 , 9 (26) . |
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Delicate modulations of CO2 activation and charge carrier separation/migration are challenging, yet imperative to augment CO2 photoreduction efficiency. Herein, by supporting diethylenetriamine (DETA)-functionalized Cd0.8Zn0.2S nanowires on the exterior surface of hollow Co9S8 polyhedrons, hierarchical Co9S8@Cd0.8Zn0.2S-DETA nanocages are fabricated as an S-scheme photocatalyst for reducing CO2 and protons to produce syngas (CO and H-2). The amine groups strengthen adsorption and activation of CO2, while the "nanowire-on-nanocage" hierarchical hollow heterostructure with an S-scheme interface boosts separation and transfer of photoinduced charges. Employing Co(bpy)(3)(2+) as a cocatalyst, the optimal photocatalyst effectively produces CO and H-2 in rates of 70.6 and 18.6 mu mol h(-1) (i.e., 4673 and 1240 mu mol g(-1) h(-1)), respectively, affording an apparent quantum efficiency of 9.45% at 420 nm, which is the highest value under comparable conditions. Ultraviolet photoelectron spectroscopy, Kelvin probe, and electron spin resonance confirm the S-schematic charge-transfer process in the photocatalyst. The key COOH* species responsible for CO2-to-CO reduction is detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and endorsed by density functional theory calculations, and thus a possible CO2 reduction mechanism is proposed.
Keyword ：
amines amines CO2 reduction CO2 reduction hollow hollow photocatalysis photocatalysis S-scheme S-scheme
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| GB/T 7714 | Su, Bo , Zheng, Mei , Lin, Wei et al. S-Scheme Co9S8@Cd0.8Zn0.2S-DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production [J]. | ADVANCED ENERGY MATERIALS , 2023 , 13 (15) . |
| MLA | Su, Bo et al. "S-Scheme Co9S8@Cd0.8Zn0.2S-DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production" . | ADVANCED ENERGY MATERIALS 13 . 15 (2023) . |
| APA | Su, Bo , Zheng, Mei , Lin, Wei , Lu, Xue Feng , Luan, Deyan , Wang, Sibo et al. S-Scheme Co9S8@Cd0.8Zn0.2S-DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production . | ADVANCED ENERGY MATERIALS , 2023 , 13 (15) . |
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