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学者姓名：陈戈
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摘要 ：
The reverse water-gas shift (RWGS) reaction holds promise for producing high value-added CO from CO2, serving as a crucial intermediate to feedstock for producing various hydrocarbons through Fischer-Tropsch synthesis reactions. Metallic catalysts often yield significant methane production as a by-product during operation, whereas non-metallic oxide catalysts offer potential for high CO selectivity. We prepare Al doped CeO2 nanorod by atomic layer deposition (ALD). The incorporation of Al creates more oxygen vacancies on the surface, resulting in increased Frustrated Lewis Pair (FLP) sites. Particularly, the CO yield of ALD-modified CeO2 was enhanced by 134 % compared to that of pristine CeO2 nanorods (CeO2-NR) at 500 degrees C, with CO selectivity reached 100 %. Density Functional Theory (DFT) calculations reveal a lower energy barrier for H2 dissociation facilitated by the formation of FLP sites, potentially leading to heightened activity in the Reverse Water Gas Shift (RWGS) reaction.
关键词 ：
Atomic layer deposition Atomic layer deposition Frustrated Lewis Pairs Frustrated Lewis Pairs CO2 hydrogenation CO2 hydrogenation RWGS reaction RWGS reaction
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| GB/T 7714 | Feng, Boyuan , Li, Shuzhen , Zhang, Long et al. Frustrated Lewis pairs on Al-doped CeO2 for efficient reverse water-gas shift reaction [J]. | APPLIED SURFACE SCIENCE , 2024 , 669 . |
| MLA | Feng, Boyuan et al. "Frustrated Lewis pairs on Al-doped CeO2 for efficient reverse water-gas shift reaction" . | APPLIED SURFACE SCIENCE 669 (2024) . |
| APA | Feng, Boyuan , Li, Shuzhen , Zhang, Long , Zhang, Guizhen , Chen, Ge . Frustrated Lewis pairs on Al-doped CeO2 for efficient reverse water-gas shift reaction . | APPLIED SURFACE SCIENCE , 2024 , 669 . |
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摘要 ：
The structure and electronic state of the active center in a single-atom catalyst undergo noticeable changes during a dynamic catalytic process. The metal atom active center is not well demonstrated in a dynamic manner. This study demonstrated that Li metal atoms, serving as active centers, can migrate on a C3N4 monolayer or between C3N4 monolayers when exposed to light irradiation. This migration alters the local coordination environment of Li in the C3N4 nanosheets, leading to a significant enhancement in photocatalytic activity. The photocatalytic H2O2 process could be maintained for 35 h with a 920 mmol/g record-high yield, corresponding to a 0.4% H2O2 concentration, which is far greater than the value (0.1%) of practical application for wastewater treatment. Density functional theory calculations indicated that dynamic Li-coordinated structures contributed to the superhigh photocatalytic activity.
关键词 ：
Oxygen reductionreaction Oxygen reductionreaction Dynamic active center Dynamic active center Coordinationenvironment Coordinationenvironment Single-atom catalyst Single-atom catalyst Photocatalytic H2O2 Photocatalytic H2O2
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| GB/T 7714 | Zhuang, Chunqiang , Chang, Yuan , Li, Weiming et al. Light-Induced Variation of Lithium Coordination Environment in g-C3N4 Nanosheet for Highly Efficient Oxygen Reduction Reactions [J]. | ACS NANO , 2024 , 18 (6) : 5206-5217 . |
| MLA | Zhuang, Chunqiang et al. "Light-Induced Variation of Lithium Coordination Environment in g-C3N4 Nanosheet for Highly Efficient Oxygen Reduction Reactions" . | ACS NANO 18 . 6 (2024) : 5206-5217 . |
| APA | Zhuang, Chunqiang , Chang, Yuan , Li, Weiming , Li, Shijie , Xu, Peng , Zhang, Hang et al. Light-Induced Variation of Lithium Coordination Environment in g-C3N4 Nanosheet for Highly Efficient Oxygen Reduction Reactions . | ACS NANO , 2024 , 18 (6) , 5206-5217 . |
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摘要 ：
The direct hydrogen peroxide (H2O2) product from H-2 and O-2 is a promising anthraquinone replacement because it is environmentally friendly and has a high atom efficiency. Experimental and theoretical studies have proven that optimizing the adsorption of the critical intermediate OOH* on the metal site significantly promotes the further protonation of this intermediate and inhibits the O-O bond cleavage, thus enhancing the activity and selectivity. Redistributing the charge density of active sites to tuning the d-band center of the metal could effectively modulate the intermediates adsorption, and thus regulate the catalytic efficiency. Herein, we show that a Lewis acid (ZnCl2 solution) induces abundant oxygen vacancies (Ovs) on the TiO2 surface, which results in a reversal of charge transfer from TiO2-Ov support to the Pd atom, generating an electron-rich Pd configuration. Compared with pristine Pd/TiO2, Pd/TiO2-Ov possesses higher H2O2 selectivity and productivity, with values of 80.7% and 186 mol kg(cat)(-1) h(-1), respectively. In addition, Pd/TiO2-Ov maintains stability during the six cycles reaction due to its high resistance to the leaching of Pd species. Theoretical calculations reveal that the reversed charge transfer downshifts the d-band center of Pd, which promotes O-2 adsorption on the Pd surface and weakens the OOH* intermediates adsorption. Thus, the energy barrier for the hydrogenation of the OOH* intermediate is significantly decreased, and the O-O band cleavage is inhibited. This study reports a reversal of charge transfer tuning the d-band center of the active site for efficient direct H2O2 synthesis, which may provide insight for designing high-performance catalysts.
关键词 ：
electronic-rich Pd surface electronic-rich Pd surface adsorption energy of OOH* adsorption energy of OOH* d-bandcenter d-bandcenter direct H2O2 synthesis direct H2O2 synthesis reversedcharge transfer reversedcharge transfer
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| GB/T 7714 | Liu, Ruilin , Wang, Chao , Yan, Yong et al. Reversed Charge Transfer to Modulate the d-Band Center of Pd for Efficient Direct H2O2 Synthesis [J]. | ACS CATALYSIS , 2024 , 14 (6) : 3955-3965 . |
| MLA | Liu, Ruilin et al. "Reversed Charge Transfer to Modulate the d-Band Center of Pd for Efficient Direct H2O2 Synthesis" . | ACS CATALYSIS 14 . 6 (2024) : 3955-3965 . |
| APA | Liu, Ruilin , Wang, Chao , Yan, Yong , Wang, Ruzhi , Chen, Ge . Reversed Charge Transfer to Modulate the d-Band Center of Pd for Efficient Direct H2O2 Synthesis . | ACS CATALYSIS , 2024 , 14 (6) , 3955-3965 . |
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摘要 ：
Stability has always been the main limiting problem for developing oxygen reduction reaction (ORR) catalysts practically. A PdZnBi alloy ORR catalyst with an interlayer-riveted carbon shell encapsulation structure is synthesized using small molecule in situ confinement effects. Meanwhile, the reaction molecular dynamics (RMD) method presents and reveals the mechanism of acetic acid molecules forming a uniform thin carbon layer on the metal surface during heat treatment. The riveted porous carbon shell structure allows rapid electron and mass transfer and acts as a protective layer that limits alloy surface oxidation and maintains the initial catalyst structure. The catalyst exhibits excellent ORR durability, with an initial mass activity (MA) of 94% after 60 000 cycles of accelerated durability tests (ADTs), and is applied to zinc-air batteries and exhibits high current density discharge stability (>100 h, 100 mA cm-2).
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| GB/T 7714 | Chang, Liyuan , Zhou, Kailing , Si, Weihan et al. In situ confined synthesis of an interlayer-riveted carbon shell encapsulated PdZnBi alloy as a highly active and durable oxygen reduction reaction catalyst [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (14) : 8194-8204 . |
| MLA | Chang, Liyuan et al. "In situ confined synthesis of an interlayer-riveted carbon shell encapsulated PdZnBi alloy as a highly active and durable oxygen reduction reaction catalyst" . | JOURNAL OF MATERIALS CHEMISTRY A 12 . 14 (2024) : 8194-8204 . |
| APA | Chang, Liyuan , Zhou, Kailing , Si, Weihan , Wang, Chao , Wang, Changhao , Zhang, Manchen et al. In situ confined synthesis of an interlayer-riveted carbon shell encapsulated PdZnBi alloy as a highly active and durable oxygen reduction reaction catalyst . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (14) , 8194-8204 . |
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摘要 ：
一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法涉及电催化领域，解决现有催化剂过电位高，选择性低，产率不足，产量无法达到工业生产水平的问题。本发明采用的是高温煅烧法，通过控制材料煅烧条件，仅改变所添加聚四氟乙烯与三聚氰胺的用量比，就能得到具有3D结构形貌的高产率低过电位的碳基催化材料，更大的相对表面积及空间个异性使得电子快速传输和逸出。元素F掺杂降低了电荷转移势垒，加速了电子‑空穴的分离和迁移，量子效率显著增加，同时改变了三相界面疏水性能，有效抑制副反应，选择性得以提升。
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| GB/T 7714 | 陈戈 , 曹会选 . 一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法 : CN202310138624.9[P]. | 2023-02-20 . |
| MLA | 陈戈 et al. "一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法" : CN202310138624.9. | 2023-02-20 . |
| APA | 陈戈 , 曹会选 . 一种用于电解水氧化合成过氧化氢的碳基催化剂的制备方法 : CN202310138624.9. | 2023-02-20 . |
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摘要 ：
一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法涉及电催化领域，解决现有合成方法步骤繁杂，控制条件多，材料不稳定，导电性能较差及产率较低等问题。本发明采用高温煅烧法制备疏水碳材料基底，采用原子层沉积法对材料进行进一步的表面改性，仅改变所沉积前驱体Ti的沉积圈数即可制备出一系列催化剂。通过F、Ti双掺杂对分子层面活性位点的调控，影响三相界面反应路径，降低电荷转移的势垒，量子效率显著增加，同时，结构致密且厚度可控的沉积层在保证催化剂电解性能的同时，对材料循环稳定性也有很大提升。出于对工业化应用中的实际需求考虑，本发明是一种原料低廉易得且结构稳定的适用于生产实践的碳基催化剂制备方法。
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| GB/T 7714 | 陈戈 , 曹会选 . 一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法 : CN202310138623.4[P]. | 2023-02-20 . |
| MLA | 陈戈 et al. "一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法" : CN202310138623.4. | 2023-02-20 . |
| APA | 陈戈 , 曹会选 . 一种基于分子尺度设计的原子层沉积法制备碳基电催化剂的方法 : CN202310138623.4. | 2023-02-20 . |
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摘要 ：
Electrocatalytic oxygen reduction reaction (ORR) for H2O2 production presents an alternative approach suitable for on-site applications. Although atomically dispersed earth-abundant metal species anchored in a nitrogen-doped carbon framework (M-N-C) have demonstrated significant 2e- ORR activity, the Ni-N-C catalyst exhibits unfavorable catalytic activity. It is well-recognized that the d-band center of the metal can be tailored by introducing transition metals, thereby altering the adsorption free energy of the OOH* reactive species. Herein, we have designed a dual-single-atom configuration (Ni-ZnNC), where the Zn atom serves as a modulator to adjust the d-band electronic energy of the Ni center, ultimately optimizing the intermediate adsorption and resulting in high 2e- ORR performance. The Ni-ZnNC catalyst demonstrates an H2O2 production rate of 5.6 mol/g/h at 0.0 VRHE with a notable H2O2 selectivity of approximately 60% in an acid electrolyte. Density-functional theory calculations reveal that the Zn atom effectively alters the d-band electronic energy of the Ni center, strengthening the Ni-OOH* binding affinity and thereby enhancing the adsorption process. This work provides valuable insights into the design of earth-abundant metal Ni-based electrocatalysts for H2O2 generation.(c) 2023 Elsevier Ltd. All rights reserved.
关键词 ：
Electronic structure Electronic structure Hydrogen peroxide production Hydrogen peroxide production Dual atomic catalyst Dual atomic catalyst ORR ORR Optimized adsorption capacity Optimized adsorption capacity
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| GB/T 7714 | Wang, Yahui , Wang, Yueshuai , Yan, Yong et al. Tailoring the d-band center of Ni on a dual-single-atom Ni-ZnNC catalyst for efficient H2O2 production [J]. | MATERIALS TODAY ENERGY , 2023 , 38 . |
| MLA | Wang, Yahui et al. "Tailoring the d-band center of Ni on a dual-single-atom Ni-ZnNC catalyst for efficient H2O2 production" . | MATERIALS TODAY ENERGY 38 (2023) . |
| APA | Wang, Yahui , Wang, Yueshuai , Yan, Yong , Yan, Lina , Cheng, Xing , Zheng, Lirong et al. Tailoring the d-band center of Ni on a dual-single-atom Ni-ZnNC catalyst for efficient H2O2 production . | MATERIALS TODAY ENERGY , 2023 , 38 . |
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摘要 ：
Developing oxide supports for stabilizing single-atom catalysts enables more flexibility for tuning the electronic metal-support interactions (EMSIs) toward better catalytic activities. However, due to the electronegativity of oxygen anions, single-metal atoms often remain positively charged in these oxide supports and are poor at binding hydrogen species for the hydrogen evolution reaction (HER). Here, we report a ligand charge donation-acquisition balance strategy via an amorphous TiBxOy support to tune the EMSIs, which lead to the boosted HER mass activity of a single Pt atom catalyst. Based on spectroscopic characterizations, we found that Pt single atoms preferentially bonded with nearly neutral B atoms originating from TiB2-like species in the Ti-B-O framework rather than O anions. Density functional theory calculations reveal that due to the charge-transfer balance between B-O and B-Pt, the nucleophilicity of Pt was tuned to an optimum state, with an ideal hydrogen binding energy that benefits the HER. As a result, this Pt/TiBxOy catalyst achieves a high HER mass activity (37.8 A mg(-1) Pt) and a turnover frequency (33.2 H-2 s(-1) Pt site(-1)) at an overpotential of 50 mV in an acid medium, outperforming commercial Pt/C by a factor of 34 and 33, respectively.
关键词 ：
single atom single atom charge transfer charge transfer amorphous support amorphous support hydrogen evolution reaction hydrogen evolution reaction electronic metal-support interactions electronic metal-support interactions
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| GB/T 7714 | Cheng, Xing , Xiao, Bo , Chen, Yanhui et al. Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction [J]. | ACS CATALYSIS , 2022 , 12 (10) : 5970-5978 . |
| MLA | Cheng, Xing et al. "Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction" . | ACS CATALYSIS 12 . 10 (2022) : 5970-5978 . |
| APA | Cheng, Xing , Xiao, Bo , Chen, Yanhui , Wang, Yueshuai , Zheng, Lirong , Lu, Yue et al. Ligand Charge Donation-Acquisition Balance: A Unique Strategy to Boost Single Pt Atom Catalyst Mass Activity toward the Hydrogen Evolution Reaction . | ACS CATALYSIS , 2022 , 12 (10) , 5970-5978 . |
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摘要 ：
一种用于直接合成过氧化氢的钯基催化剂的制备方法属于多相催化领域，是用于以氢气和氧气为原料直接合成过氧化氢的新型钯基催化剂的方法。直接合成过氧化氢中现有的催化剂都是钯纳米颗粒，且过氧化氢产率和选择性一直很低。本发明的催化剂为二氧化钛负载的钯单原子，且贵金属钯的负载量仅为0.1wt％。该催化剂是通过将四氯钯酸钠前驱体添加到二氧化钛悬浮液中，待浸渍后离心洗涤得到。当用于以氢气和氧气为原料直接合成过氧化氢时，该催化剂的过氧化氢产率为115mol/kgcat/h，选择性大于99％，超过了以往专利报道的最高值，具有良好的工业应用前景。
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| GB/T 7714 | 陈戈 , 余世明 , 于涵 . 一种用于直接合成过氧化氢的钯基催化剂的制备方法 : CN202210168066.6[P]. | 2022-02-23 . |
| MLA | 陈戈 et al. "一种用于直接合成过氧化氢的钯基催化剂的制备方法" : CN202210168066.6. | 2022-02-23 . |
| APA | 陈戈 , 余世明 , 于涵 . 一种用于直接合成过氧化氢的钯基催化剂的制备方法 : CN202210168066.6. | 2022-02-23 . |
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摘要 ：
一种湿法制备铂基贵金属催化剂的方法属于多相催化领域，提供一种适用于工业化，绿色环保的高活性铂基催化剂的制备方法。用来克服现有合成方法步骤复杂，控制条件多，现有商业化铂基催化剂铂原子利用率低的缺点。本方法采用简单水热法，将前驱体的载体粉末合成前驱体材料，在采用管式炉在多种气体中煅烧最后进行研磨，造粒等操作得到高活性的Pt基催化剂材料。该材料在标准的一氧化碳氧化条件下，可以在90℃的低温条件下达到100％的一氧化碳氧化效率。此合成方法采用简单水热法合成，过于复杂的贵金属合成路线，提高了原材料的利用效率，降低了合成的成本，合成过程简单，是一条绿色简易的湿法合成路线，适用于工业大规模生产。
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| GB/T 7714 | 陈戈 , 于涵 , 余世明 . 一种湿法制备铂基贵金属催化剂的方法 : CN202210168088.2[P]. | 2022-02-23 . |
| MLA | 陈戈 et al. "一种湿法制备铂基贵金属催化剂的方法" : CN202210168088.2. | 2022-02-23 . |
| APA | 陈戈 , 于涵 , 余世明 . 一种湿法制备铂基贵金属催化剂的方法 : CN202210168088.2. | 2022-02-23 . |
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