ORCID Profile
0000-0002-8256-6053
Current Organisation
Northeastern University
Does something not look right? The information on this page has been harvested from data sources that may not be up to date. We continue to work with information providers to improve coverage and quality. To report an issue, use the Feedback Form.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2CP05959B
Abstract: Based on first-principles calculations, we designed a highly effective SiM@C 3 N 4 catalyst as the low-cost candidate for electrocatalytic ammonia synthesis.
Publisher: American Chemical Society (ACS)
Date: 22-10-2018
Publisher: Elsevier BV
Date: 09-2021
Publisher: Wiley
Date: 15-09-2020
Publisher: Wiley
Date: 2023
Abstract: The room‐temperature nitrogen reduction reaction (NRR) is of paramount significance for both the fertilizer industry and fundamental catalysis science. To produce ammonia from water, air, and sunlight, the photocatalytic NRR is targeted to significantly release the energy and environmental pressure associated with the current Habor–Bosch process. In this context, herein, the knowledge‐driven design of boron‐doped TiO 2 is demonstrated as a photocatalyst for the nitrogen reduction reaction. Among 54 catalysts in the reported library, anatase TiO 2 (101) modified by boron doping is identified as an exceptional NRR catalyst with strong visible‐light absorption (bandgap 1.92 eV) and excellent reactivity with a small thermodynamic barrier (0.44 eV) as well as a high turnover frequency (1.08 × 10 −5 s −1 site −1 ). Experimentally, the predictions of this work are validated using a B‐doped TiO 2 nanosheet, achieving ammonia production with a yield of 3.35 mg h −1 g −1 under simulated sunlight irradiation, which significantly renews the performance record for Ti‐based photocatalyst for the NRR. This work highlights the importance of dual active site catalysts for nitrogen activation and reduction and demonstrates the capacity of knowledge‐driven catalyst design.
Publisher: Wiley
Date: 21-04-2020
Publisher: Wiley
Date: 29-10-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9TA10346E
Abstract: A Ru 2 P–reduced graphene oxide hybrid acts as a superior catalyst for electrochemical N 2 fixation in 0.1 M HCl, achieving a large NH 3 yield of 32.8 μg h −1 mg cat. −1 and a high faradaic efficiency of 13.04%−0.05 V vs. the reversible hydrogen electrode.
Publisher: American Chemical Society (ACS)
Date: 05-02-2019
DOI: 10.1021/JACS.8B13165
Abstract: Boron has been explored as p-block catalysts for nitrogen reduction reaction (NRR) by density functional theory. Unlike transition metals, on which the active centers need empty d orbitals to accept the lone-pair electrons of the nitrogen molecule, the sp
Publisher: Wiley
Date: 26-03-2022
Abstract: Recognizing and controlling the structure–activity relationships of single‐atom catalysts (SACs) is vital for manipulating their catalytic properties for various practical applications. Herein, Fe SACs supported on nitrogen‐doped carbon (SA‐Fe/CN) are reported, which show high catalytic reactivity (97% degradation of bisphenol A in only 5 min), high stability (80% of reactivity maintained after five runs), and wide pH suitability (working pH range 3–11) toward Fenton‐like reactions. The roles of different N species in these reactions are further explored, both experimentally and theoretically. It is discovered that graphitic N is an adsorptive site for the target molecule, pyrrolic N coordinates with Fe(III) and plays a dominant role in the reaction, and pyridinic N, coordinated with Fe(II), is only a minor contributor to the reactivity of SA‐Fe/CN. Density functional theory (DFT) calculations reveal that a lower d‐band center location of pyrrolic‐type Fe sites leads to the easy generation of Fe‐oxo intermediates, and thus, excellent catalytic properties.
Publisher: American Chemical Society (ACS)
Date: 04-01-2019
Publisher: Wiley
Date: 13-06-2021
Abstract: 2D bismuth nanosheets are a promising layered material for formate‐producing via electrocatalytic CO 2 conversion. However, the commercial interest of bismuth nanosheets in CO 2 electroreduction is still rare due to the undesirable current density for formate at moderate operation potentials (about 200 mA mg −1 ) and harsh synthesis conditions (high temperature and/or high pressure). This work reports the preparation of Bi nanosheets with a lateral size in micrometer‐scale via electrochemical cathodic exfoliation in aqueous solution at normal pressure and temperature. As‐prepared Bi LNSs (L indicates large lateral size) possess high Faradaic efficiencies over 90% within a broad potential window from −0.44 to −1.10 V versus RHE and a superior partial current density about 590 mA mg −1 for formate in comparison with state‐of‐the‐art results. Structure analysis, electrochemical results, and density functional theory calculations demonstrate that the increasing tensile lattice strain observed in Bi LNSs leads to less overlap of d orbitals and a narrower d‐band width, which tuning the intermediate binding energies, and therefore promotes the intrinsic activity.
Publisher: Wiley
Date: 19-08-2022
Abstract: Transition‐metal‐mediated dinitrogen fixation has been intensively investigated. The employment of main group elements for this vital reaction has recently sparked interest because of new dinitrogen reaction chemistry. We report ammonia synthesis via a chemical looping process mediated by a transition‐metal‐free barium hydride (BaH 2 ). Experimental and computational studies reveal that the introduction of hydrogen vacancies is essential for creating multiple coordinatively unsaturated Ba sites for N 2 activation. The adjacent lattice hydridic hydrogen (H − ) then undergoes both reductive elimination and reductive protonation to convert N 2 to NH x . The ammonia production rate supports this hydride‐vacancy mechanism via a chemical looping route that far exceeds that of a catalytic process. The BaH 2 ‐mediated chemical looping process has prospects in future technologies for ammonia synthesis using transition‐metal‐free materials.
Publisher: Elsevier BV
Date: 04-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9MH01668F
Abstract: This review provides an up-to-date review on Bi-based nitrogen-fixation materials and future directions for the development of new Bi-based nitrogen-fixation materials under ambient conditions.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8TA08219G
Abstract: By first-principles computations, nitrogen becomes activated via distal pathway on the single Ru-atom-embedded two boron monolayers, exhibiting relatively low reaction energy barriers of 0.42 and 0.44 eV, respectively.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2NR01551J
Abstract: An efficient metal free carbon-based electrocatalyst is prepared for nitrogen reduction.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0NJ04068A
Abstract: Defective g-C 3 N 4 nanorods enable to boots the adsorption and cleavage of N 2 molecules to achieve higher photocatalytic nitrogen fixation performance.
Publisher: MDPI AG
Date: 11-09-2021
Abstract: Benefitting from a suitable band gap, ceria is an excellent material for UV shielding. By solid solution doping and specific micromorphology, its band gap can be effectively controlled. In this paper, ceria doped with lanthanum via oxalate precipitation is combined with a high-temperature roasting process. The properties of the prepared s les are characterized by UV–Vis diffuse reflectance spectroscopy (DRS), Raman, XRD, FESEM and XPS. The absorption threshold of materials is clearly red-shifted in the ultraviolet band, which originates from the electron-phonon generation. To further reveal the mechanism, the density function theory calculation (DFT) is implemented to study the influence of lanthanum concentrations on ceria’s band gap. It is demonstrated that the band gap can even be narrowed to 2.97 eV by optimizing the sintering temperature and lanthanum-doped concentration. To investigate its improved anti-aging properties under ultraviolet rays, different amounts of 5% lanthanum-doped ceria is mixed with an Al-based coating and then coated on the Q235 steel. Combined with an ultraviolet light irradiation experiment and electrochemical test technology, the corrosion resistance of the modified coatings is evaluated. The coating with 20% La-doped ceria provides the best corrosion resistance performance.
Publisher: Elsevier BV
Date: 08-2021
Publisher: Wiley
Date: 16-12-2023
Abstract: Environmentally friendly ammonia production is important for addressing the carbon emissions and substantial energy consumption that are currently associated with the chemical industry. In recent decades, many achievements are made in this area however, low production yield, poor selectivity, and unsatisfactory Faradaic efficiency hinder large‐scale applications. 2D, metal‐free electrocatalysts stand out from other candidates because of their physical, electronic, and chemical properties. In this study, recent developments of 2D‐based electrochemical materials for converting dinitrogen into ammonia in ambient conditions are systematically reviewed. First, recent unique progress and challenges on novel 2D electrocatalysts for the nitrogen reduction reaction are summarized. Then, various synthetic strategies for electrochemical materials and the influence of these methods have on the intrinsic material performance are highlighted. Last, by comparing current engineering strategies, electrochemical tests, and computational calculations, the opportunities, critical issues, and scientific challenges for 2D nanomaterials as stable, efficient catalysts, are analyzed. On the basis of this comparison, technology solutions are provided and rational principles for future studies are proposed.
Publisher: Elsevier BV
Date: 05-2022
Publisher: American Chemical Society (ACS)
Date: 26-07-2018
Publisher: Wiley
Date: 30-06-2023
Abstract: Electrocatalytic nitrogen reduction reaction ( e NRR) relies on developing efficient catalysts towards high reaction activity and selectivity. In recent years, designing single‐atom catalysts have been the research frontier in electrochemical reactions. However, compared to their widely studied applications in oxygen electrocatalysis, their potential structure‐function relationship and reaction mechanism in e NRR were less explored. Herein, single‐atom Fe−N x −C materials were systematically analysed considering the coordination environments of single‐atom Fe. It was found that coordination environment plays a key role in determining the N 2 adsorption and activation. Among the concept catalysts designed, FeCN 2 and FeCN 3 offer the highest e NRR activities with a suppressed side reaction ( i. e ., the hydrogen evolution). Moreover, the Bader charge of the single‐atom Fe and *NH adsorption energy can be the good descriptors to guide the design of e NRR catalysts. This study unravels the key role of coordination environment in tuning the reactivity of e NRR over single‐atom Fe−N x −C materials.
Publisher: Elsevier BV
Date: 05-2022
Publisher: American Chemical Society (ACS)
Date: 07-12-2021
Publisher: American Chemical Society (ACS)
Date: 23-03-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9TA04650J
Abstract: Iron hypercoordinated with boron is a promising catalyst for the nitrogen reduction reaction.
Publisher: Elsevier BV
Date: 04-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC04789F
Abstract: A solid-solution nanoalloy of bulk-immiscible CuAg synthesized by far-from-equilibrium electrochemical reduction from the parent oxide exhibits enhanced tandem catalysis for CO 2 reduction.
No related grants have been discovered for Chuangwei Liu.