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154. p-d orbital hybridization induced by CuGa2promotes selective N2electroreduction

Author

Chen, Bin, Zheng, Chaoyang, Shi, Dehuan, Huang, Yi, Deng, Renxia, Wei, Yang, Liu, Zheyuan, Yu, Yan, and Zhong, Shenghong

Abstract

In the quest to align with industrial benchmarks, a noteworthy gap remains in the field of electrochemical nitrogen fixation, particularly in achieving high Faradaic efficiency (FE) and yield. The electrocatalytic nitrogen fixation process faces considerable hurdles due to the difficulty in cleaving the highly stable N≡N triple bond. Additionally, the electrochemical pathway for nitrogen fixation is often compromised by the concurrent hydrogen evolution reaction (HER), which competes aggressively for electrons and active sites on the catalyst surface, thereby reducing the FE of nitrogen reduction reaction (NRR). To surmount these challenges, this study introduces an innovative bimetallic catalyst, CuGa2, synthesized through p-d orbital hybridization to selectively facilitate N2electroreduction. This catalyst has demonstrated a remarkable NH3yield of 9.82 μg h−1 cm−2and an associated FE of 38.25%. Our findings elucidate that the distinctive p-d hybridization interaction between Ga and Cu enhances NH3selectivity by reducing the reaction energy barrier for hydrogenation and suppressing hydrogen evolution. This insight highlights the significance of p-d orbital hybridization in optimizing the electrocatalytic performance of CuGa2for nitrogen fixation.

Published
2025
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155. Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2reduction by targeted electron transport

Author

Ning, Jiangqi, Huang, Junhan, Liu, Yuhang, Chen, Yanlei, Niu, Qing, Lin, Qingqing, He, Yajun, Liu, Zheyuan, Yu, Yan, and Li, Liuyi

Abstract

Targeted electron transfer to catalytically active site for CO2reduction is promising for enhancing the efficiency of artificial photosynthesis. Here, we demonstrate a design of an alkyl-linked heterostructure composing of TiO2and a Cu-porphyrin-based covalent organic framework (TiO2@CuPorTT-COF) for the photoreduction of CO2with H2O. Through specific coordination effect, the alkyl chain bridges TiO2and Cu moiety in COF. Upon light illumination, the photoinduced electrons in TiO2can be directionally transported across the interface along the alkyl chain to the Cu active sites to reduce adsorbed CO2, while the left holes are consumed by the H2O oxidation, enhancing the spatial separation and utilization of electron-hole pairs. Accordingly, the TiO2@CuPorTT-COF enables remarkably superior catalytic activities over the counterpart without the alkyl bridge for electron transfer with 5 times of CO production rate. An apparent quantum efficiency of 0.455% at 380 nm is achieved. Moreover, a dynamic evolution of Cu active site for CO2reduction is revealed, which can be promoted by the targeting electron transport approach. This work provides a targeted electron transport strategy for constructing photocatalysts.

Published
2024
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165. Establishing the carrier scattering phase diagram for ZrNiSn-based half-Heusler thermoelectric materials

Author

Ren, Qingyong, primary, Fu, Chenguang, additional, Qiu, Qinyi, additional, Dai, Shengnan, additional, Liu, Zheyuan, additional, Masuda, Takatsugu, additional, Asai, Shinichiro, additional, Hagihala, Masato, additional, Lee, Sanghyun, additional, Torri, Shuki, additional, Kamiyama, Takashi, additional, He, Lunhua, additional, Tong, Xin, additional, Felser, Claudia, additional, Singh, David J., additional, Zhu, Tiejun, additional, Yang, Jiong, additional, and Ma, Jie, additional

Published
2020
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169. A high-pressure visual flow loop for hydrate blockage detection and observation

Author

Lei Yang, Liu Zheyuan, Jiafei Zhao, Bo Xiao, Hanquan Zhang, and Mingjun Yang

Subjects
010302 applied physics, Petroleum engineering, business.industry, Multiphase flow, Clathrate hydrate, Flow (psychology), 01 natural sciences, 010305 fluids & plasmas, Pipe flow, Pipeline transport, Natural gas, 0103 physical sciences, Environmental science, Deposition (phase transition), Hydrate, business, Instrumentation
Abstract

More than 65% of the worldwide natural gas is transported through pipelines. Gas hydrate formation and blockage in the pipeline are commonly encountered, causing significant problems in safe and efficient transportation. Yet the instrument simulating the high-pressure multiphase flow and demonstrating the hydrate blocking behavior at flowing conditions is not available. In this work, a high-pressure visual flow loop is developed to detect and observe the hydrate nucleation, growth, and deposition during the multiphase flow. The pressure limit is designed to be 8 MPa, and the temperature can go down to −20 °C. This device allows a direct observation of the gas-liquid flow regime during transportation; investigations on the initiation and evolution of hydrate blockage in the dead-leg section, U-shaped region, and rising pipes are now possible. Sensors are distributed along the pipelines to detect the pressure and temperature change; the differential pressure is used to effectively detect the degree of hydrate blockage, which increases upon hydrate formation. The visual flow loop could also help examine the effect of shut-down and restart of the pump on the flow behavior. The system has been verified feasible demonstrating the flow behavior and predict hydrate blockage. The developed device would help understand the mechanism of hydrate blockage in the transportation pipelines and provide guidance to efficiently avoid such problems.More than 65% of the worldwide natural gas is transported through pipelines. Gas hydrate formation and blockage in the pipeline are commonly encountered, causing significant problems in safe and efficient transportation. Yet the instrument simulating the high-pressure multiphase flow and demonstrating the hydrate blocking behavior at flowing conditions is not available. In this work, a high-pressure visual flow loop is developed to detect and observe the hydrate nucleation, growth, and deposition during the multiphase flow. The pressure limit is designed to be 8 MPa, and the temperature can go down to −20 °C. This device allows a direct observation of the gas-liquid flow regime during transportation; investigations on the initiation and evolution of hydrate blockage in the dead-leg section, U-shaped region, and rising pipes are now possible. Sensors are distributed along the pipelines to detect the pressure and temperature change; the differential pressure is used to effectively detect the degree of hydra...

Published
2019

172. High-mobility organic single-crystalline transistors with anisotropic transport based on high symmetrical “H”-shaped heteroarene derivatives

Author

Fan, Hanghong, primary, Zou, Sufen, additional, Gao, Jianhua, additional, Chen, Ru, additional, Ma, Qingfang, additional, Ma, Wangjing, additional, Zhang, Huarong, additional, Chen, Guangjin, additional, Huo, Xinwei, additional, Liu, Zheyuan, additional, Dang, Yanfeng, additional, and Hu, Wenping, additional

Published
2020
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176. Organic Single Crystals: A “Phase Separation” Molecular Design Strategy Towards Large‐Area 2D Molecular Crystals (Adv. Mater. 35/2019)

Author

Fu, Beibei, primary, Wang, Cong, additional, Sun, Yantao, additional, Yao, Jiarong, additional, Wang, Yu, additional, Ge, Fayuan, additional, Yang, Fangxu, additional, Liu, Zheyuan, additional, Dang, Yanfeng, additional, Zhang, Xiaotao, additional, Shao, Xiangfeng, additional, Li, Rongjin, additional, and Hu, Wenping, additional

Published
2019
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180. Density Functional Theory Mechanistic Insight into the Base-Free Nickel-Catalyzed Suzuki–Miyaura Cross-Coupling of Acid Fluoride: Concerted versus Stepwise Transmetalation

Author

Zhang, Chaoshen, Zhao, Ruihua, Dagnaw, Wasihun Menberu, Liu, Zheyuan, Lu, Yu, Wang, Zhi-Xiang, Zhang, Chaoshen, Zhao, Ruihua, Dagnaw, Wasihun Menberu, Liu, Zheyuan, Lu, Yu, and Wang, Zhi-Xiang

Abstract

Density functional theory mechanistic study has been carried out to account for the base-free nickel-catalyzed Suzuki-Miyaura coupling of acid fluorides (ArC(O)F) with boronic acids (Ar'B(OH)(2)). After oxidative addition to break the C-F bond of acid fluoride, the resultant ArC(O)[Ni]F species undergoes transmetalation with Ar'B-(OH)(2) to give ArC(O)[Ni]Ar'. Subsequently, ArC(O)[Ni]Ar' can either undergo decarbonylation, finally leading to the coupling product (ArAr'), or reductive elimination to give ketone byproduct ArC(O)Ar'. The kinetic competition between the two pathways controls the chemoselectivity of the reaction, and transmetalation is the rate-determining step of the coupling. Importantly, it was found that transmetalation prefers a stepwise mechanism over a conventional concerted one. Detailed analyses indicate that the strong fluorophilicity of boron facilitates the base-free transmetalation and the coordination interaction between an oxygen atom of boronic acid and nickel gears the base-free transmetalation to undergo the stepwise pathway. The stepwise transmetalation mechanism also involves the nickel-catalyzed Suzuki-Miyaura coupling of aldehydes with ketone (PhC(O)CF3) as the transmetalation promoter.

Published
2019

181. Nitrogen–nitrogen-functionalized N-heterocyclic carbene ruthenium(ii) complexes realized efficient CO2hydrogenation to formateElectronic supplementary information (ESI) available. CCDC 2125582, 2125759and 2125625. For ESI and crystallographic data in CIF or other electronic format see DOI: https://doi.org/10.1039/d2cy00741j

Author

Gong, Huihua, Cui, Tianhua, Liu, Zheyuan, Zheng, Yanling, Zheng, Xueli, Fu, Haiyan, Yuan, Maolin, Chen, Hua, Xu, Jiaqi, and Li, Ruixiang

Abstract

Three novel Ru(ii)–CNN complexes, namely, [RuH(CO)(PPh3)2(κ2-NimN)]Cl2(1), [fac-RuH(CO)(PPh3)(κ3-CNHN)]Cl (2) and [fac-RuH(CO)(PPh3)(κ3-CNMeN)]Cl (3), have been synthesized for efficient CO2hydrogenation to formate. Complex 2bearing a CNHN ligand exhibits excellent activity and a long catalytic lifetime of 400 h at 170 °C. Notably, the addition of PPh3leads to increased activity and gives a high TON of 6.5 × 105after 400 h.

Published
2022
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190. Novel Inorganic‐Organic Dual‐Photosensitizing Dinuclear‐Metal Self‐Assembly System for Efficient Artificial Photosynthesis without Sacrificial Electron Donors.

Author

Wang, Jiaxin, Song, Tianqun, Liu, Zheyuan, Yun, Qinbai, Sun, Juehan, Zhang, Ying, Yuan, Kuo, Zhong, Dichang, Tang, Zhiyong, and Lu, Tongbu

Abstract

Owing to the unique synergistic effect, dinuclear‐metal‐molecule‐catalysts (DMCs) show excellent performance in catalytic fields. However, for overall photocatalytic CO2 reaction (CO2RR), it is still a challenge to construct well‐matched photosensitizer (PS) components for DMCs‐based photocatalysts. Inorganic‐quantum‐dot PS possesses capacities of multiple exciton generation and catalyzing water oxidation but is incompatible with DMCs. In contrast, organic PS can be covalently linked with DMCs but inescapable of using sacrificial electron donors. For overall photocatalytic CO2RR, organic–inorganic dual‐photosensitizing system might be a promising candidate. Herein, we employed covalent‐linking and electrostatic‐driven approaches to construct the self‐assembly of pyrene‐sensitized Co2L DMCs (Py‐Co2L) and perovskite (PVK) quantum dots, i.e., PVK@[Py‐Co2L]. Using H2O as an electron donor, PVK@[Py‐Co2L] realized 105.24 μmol ⋅ g−1⋅h−1 CO yield in photocatalytic CO2RR, much higher than PVK (15.44 μmol ⋅ g−1⋅h−1) and PVK@Co2L (32.30 μmol ⋅ g−1 ⋅ h−1), ascribing to the efficient photogenerated charge separation and transfer. The experimental results and theoretical investigations demonstrated that the pyrene linked on Co2L boosted the electron delivery from PVK to DMCs. Besides, this strategy could also be extended to the photocatalytic H2 evolution coupled with alcohol oxidation. As a proof‐of‐concept, our work lightens the integration of DMCs, organic and inorganic PS components, promoting the development of photocatalysis without sacrificial electron donors. [ABSTRACT FROM AUTHOR]

Published
2024
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192. Phase I study of injectable, depot naltrexone for the relapse prevention treatment of opioid dependence

Author

Wang Xu-yi, Wang Juelu, Xiang Xiao-jun, Gong Zhehui, Liu Gang, Hao Wei, Dong Guoming, Li Haiyan, Li Jin, and Liu Zheyuan

Subjects
Depot, business.industry, Medicine (miscellaneous), Relapse prevention, Placebo, Naltrexone, Psychiatry and Mental health, Clinical Psychology, Pharmacokinetics, Tolerability, Opioid, Anesthesia, medicine, Adverse effect, business, medicine.drug
Abstract

Background and Objectives We tested long-acting injectable depot naltrexone for its tolerability, pharmacokinetics, and safety in Phase I. Methods The Phase I trial enrolled 36 healthy participants in two panels (A, B). In Panel A, 24 subjects were randomly assigned to the high-dosage group (400 mg naltrexone, n = 6; placebo, n = 6) or low-dosage group (200 mg naltrexone, n = 6; placebo, n = 6). In Panel B, 12 subjects were randomized to take six doses of monthly injectable naltrexone (400 mg) or placebo. Results After a single injection of naltrexone 200 and 400 mg, means (SD) of naltrexone plasma concentrations were .57 (.28) ng/ml and 1.5 (.8) ng/ml 30 days post-injection. There was no effect of accumulation after multiple dosing. Eleven of 30 subjects (36.67%) who were administered injectable depot naltrexone reported a total of 12 adverse events (AEs). Seven of these 11 AEs were coded as possibly related with study medication. All treatment-related AEs were mild in severity. No serious treatment-related AEs occurred. Discussion and Conclusions This long-acting formulation of injectable depot naltrexone is well tolerated, results in constant plasma concentration of naltrexone for at least 1 month. Scientific Significance The tolerability and safety of long-acting injectable depot naltrexone are good. (Am J Addict 2014;23:162–169)

Published
2013
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199. Dynamic prediction of interface level using spatial temporal markov random field.

Author

Liu, Zheyuan, Kodamana, Hariprasad, Afacan, Artin, and Huang, Biao

Subjects
*MARKOV random fields, *MARKOV processes, *OIL sands, *IMAGE segmentation, *GAUSSIAN mixture models, *ECONOMIC forecasting
Abstract

Maintaining a desired interface level plays a key role for the efficient extraction in oil sands, mining and related industries. However, varying throughputs and downstream disturbances tend to change the interface level over time. Hence, measurement of the interface level is an important indicator of the process behavior and is useful for economical operation and improved control. In this paper, we propose a Spatial Temporal Markov Random Field (ST-MRF) based image segmentation approach for the dynamic prediction of the interface level. We assume that interface level, which is modeled as MRF, propagates as a Markov chain across time, yielding a ST-MRF model. The proposed approach is validated using the images captured from laboratory scale equipment designed to simulate the industrial scenarios. [ABSTRACT FROM AUTHOR]

Published
2019
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