Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

Huang, Libei; Cheng, Le; Ma, Tinghao; Zhang, Junjie; Wu, Haikun; Su, Jianjun; Song, Yun Mi; Zhu, He; Liu, Qi; Zhu, Minghui; Zeng, Zhiyuan; He, Qiyuan; Tse, Man‐Kit; Yang, Deng‐Tao; Yakobson, Boris I.; Tang, Ben Zhong; Ren, Yang; Ye, Ruquan

doi:10.1002/adma.202211856

Cited by 61 publications

(42 citation statements)

References 80 publications

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“…For example, the presence of the structural defects can tune the charge localization on the carbon and also the coordination between the metal center and the carbon host. 27,52,53 The exact local bonding configuration and coordination of La can be tuned by enlarging the vacancies in graphene, which provides more flexibility for introducing additional functional groups. 27,52 In addition, the reaction mechanism may vary depending on the active sites as the latter determines the stability of different species over the surface, such as NOH on metal-free but defect-rich graphene 53 and HNO over the metal and Co-SAC.…”

Section: Resultsmentioning

confidence: 99%

Lanthanum-Doped Graphene for Electrocatalytic Reduction of Nitrogen Monoxide

2023

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Electrocatalytic conversion of nitrogen oxides is a promising approach to address nitrogen pollution in underground water. Nitrogen oxides, such as nitrate and nitrite, can be reduced to N 2 and NH 3 over an electrocatalyst, with NO as the key intermediate, subsequent reaction of which controls the overall activity and selectivity. Here, we report density functional theory calculations of NO electrocatalytic reduction (NOER) over lanthanum embedded in graphene, through which we show that the localized states in La drive the reaction favorably due to more pronounced molecular adsorption and charge transfer than transition metals such as Co. The free energy profiles are compared between the La-based single-atom catalyst (SAC) and Co-based SAC, for producing N 2 and NH 3 . We find that the La-SAC intensifies the electron transfer to the adsorbed NO, promoting the first protonation step of NO, which is the potential-limiting step on the Co-SAC. Also, an intriguing effect of the water solvent is revealed on the La-SAC. In addition to stabilizing the intermediate species, water molecules that are coordinated with La participate directly in the protonation steps, enhancing the catalyst activity. This study reveals the unique mechanism of NOER over rare-earth-based catalysts, highlighting the potential application of atomically dispersed f-block elements for electrocatalytic reactions.

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Section: Resultsmentioning

confidence: 99%

Lanthanum-Doped Graphene for Electrocatalytic Reduction of Nitrogen Monoxide

2023

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“…This is partly related to poor repeatability of bioderived materials or to incomplete characterization and description of materials and processing in some studies. Instead, the atomic structure and the morphology , of synthetic precursors can be more easily characterized and tuned for the specific application, enhancing LIG performance. However, this leads to an increase in costs and has an effect on the overall sustainability of the process.…”

Section: Discussionmentioning

confidence: 99%

Bioderived Laser-Induced Graphene for Sensors and Supercapacitors

Bressi,

Dallinger,

Steksova

et al. 2023

ACS Appl. Mater. Interfaces

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The maskless and chemical-free conversion and patterning of synthetic polymer precursors into laser-induced graphene (LIG) via laser-induced pyrolysis is a relatively new but growing field. Bioderived precursors from lignocellulosic materials can also be converted to LIG, opening a path to sustainable and environmentally friendly applications. This review is designed as a starting point for researchers who are not familiar with LIG and/or who wish to switch to sustainable bioderived precursors for their applications. Bioderived precursors are described, and their performances (mainly crystallinity and sheet resistance of the obtained LIG) are compared. The three main fields of application are reviewed: supercapacitors and electrochemical and physical sensors. The key advantages and disadvantages of each precursor for each application are discussed and compared to those of a benchmark of polymer-derived LIG. LIG from bioderived precursors can match, or even outperform, its synthetic analogue and represents a viable and sometimes better alternative, also considering its low cost and biodegradability.

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“…43 Additionally, lattice defects present in LIG have been found to induce higher electrocatalytic properties. 44 The advantage of high electrochemical performance and scalable fabrication process has allowed the detection of pollutants of environmental significance. 37,40,45−47 The nitro group in 4-NP is susceptible to redox changes by heterogeneous electron transfer in the presence of external potential.…”

Section: Introductionmentioning

confidence: 99%

Dual Linear Range Laser-Induced Graphene-Based Sensor for 4-Nitrophenol Detection in Water

Wanjari

Duttagupta

Singh

2023

ACS Appl. Nano Mater.

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Electrochemical sensors provide an excellent platform for in situ water pollutant detection. Graphene-based electrochemical sensors have been effective in the analysis of different genres of pollutants. However, the complex, chemically intensive steps of graphene fabrication and its modification pose challenges to the large-scale application of these sensors. Laser-induced graphene (LIG) is a promising technology with a simple, rapid, chemical-free, mask-free, and scalable solution to produce graphene-based electrochemical sensors. Among a diverse array of water pollutants, 4-nitrophenol (4-NP) is a critical pollutant owing to its acute toxicity and adverse health effects on humans and other living organisms. It is known to have carcinogenic, mutagenic, and teratogenic effects on aquatic life, plants, and human beings at very low concentrations. This work demonstrated a simple nonreceptor-based electrochemical sensor for 4-NP detection by laser-induced graphene (LIG) printed on polyimide (PI) films. The laser irradiation of polymeric films results in 3D porous graphene structure formation, which increases the electron transfer rate as well as the electrochemically active surface area. The LIG sensor was fabricated by optimizing laser settings and characterized by SEM, TEM, XRD, Raman spectroscopy, XPS, TGA, and EDS analysis. Using linear sweep voltammetry, the LIG sensors demonstrated linear behavior in two concentration ranges from 0.15 to 1 μM and 2.5 to 100 μM with a detection limit of 95 nM. A higher sensitivity was observed for the lower concentration range, which could be attributed to increased electrochemical sites for 4-NP in the porous LIG. The sensor showed good selectivity toward 4-NP in the presence of its isomers and other phenolic compounds. Furthermore, it showed good selectivity in sewage samples spiked with different 4-NP concentrations. The enhanced sensitivity of LIG toward 4-NP at a lower concentration range could pave the way for high-performance sensors using LIG for environmental and other applications.

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Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

Cited by 61 publications

References 80 publications

Lanthanum-Doped Graphene for Electrocatalytic Reduction of Nitrogen Monoxide

Lanthanum-Doped Graphene for Electrocatalytic Reduction of Nitrogen Monoxide

Bioderived Laser-Induced Graphene for Sensors and Supercapacitors

Dual Linear Range Laser-Induced Graphene-Based Sensor for 4-Nitrophenol Detection in Water

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