In-situ polymerization induced atomically dispersed manganese sites as cocatalyst for CO2 photoreduction into synthesis gas

Yang, Jia; Wang, Zhiyuan; Jiang, Jianchao; Chen, Wenxing; Liao, Fan; Ge, Xin; Zhou, Xiao Yan; Chen, Min; Li, Ruilong; Xue, Zhenggang; Wang, Gang; Duan, Xuezhi; Zhang, Guoqing; Wang, Yang‐Gang; Wu, Yuen

doi:10.1016/j.nanoen.2020.105059

Cited by 62 publications

(42 citation statements)

References 33 publications

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“…The MnO 2 nanowires were used as sacrificial template, and its gradual dissolution initiated the simultaneous interfacial polymerization of pyrrole and aniline, generating coaxial crosslinked polyaniline-polypyrrole@MnO 2 (PANi-PPy@MnO 2 ) nanostructure with uniform polymer wrapping shells (Figures 1b and S2). [40][41][42] The redox reaction between oxidant and monomer can be expressed by following:…”

Section: Methodsmentioning

confidence: 99%

“…The presence of Mn 2+ cations could catalyze the graphitization as discussed in the literature where metal cations (e.g., Fe 3+ , Mn 2+ ) embedded in carbon precursor could facilitate the catalytic graphitization process. 41,[43][44][45] The resulted carbothermal Page 8 of 26 CCS Chemistry reaction rendered the formation of expanded nanographite and multipores with the simultaneous incorporation of heteroatom and Lewis acid doping of N and Mn into the carbon matrix. 41,46 The pyrolyzed product was washed with acid to remove loosely attached Mn components including MnO x and Mn clusters, and a second thermal activation process was employed to repair the structure of MnN 4 into atomically dispersed single atom catalysts and increase the Mn-doping content, producing the best-performance LA-2MnNC hollow nanorod catalysts (the same as above, refers to the molar ratio between aniline and pyrrole monomers).…”

Section: Methodsmentioning

confidence: 99%

“…The Mn K-edge X-ray absorption near-edge structure (XANES) spectrum of the LA-2MnNC catalyst exhibited a threshold energy between Mn (II) O and Mn (IV) O 2 and was very close to that of well-defined MnN 4 structure in MnPc (Figure 2a), which is in line with TEM results and suggests the strong coupling Mn-N interaction with Mn close to the 2+ oxidation state. 41,45 The Figure 2b compares the Fourier transform (FT) k 2weighted extended X-ray absorption fine structure (EXAFS) spectra of the LA-2MnNC catalyst with standard references. The strongest contribution and a hump are presented at c.a.…”

Section: Methodsmentioning

confidence: 99%

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Atomically Dispersed Manganese Lewis Acid Sites Catalyze Electrohydrogenation of Nitrogen to Ammonia

Shang

Song

et al. 2022

CCS Chem

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Ambient electrochemical nitrogen fixation is a promising and environmentally benign route for producing sustainable ammonia, but has been limited by poor performance of existing catalysts that promote the balanced chemisorption of N 2 and subsequent electrochemical activation and hydrogenation. Herein, we describe the highly selective and efficient electrohydrogenation of nitrogen to ammonia using hollow nanorod-

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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Atomically Dispersed Manganese Lewis Acid Sites Catalyze Electrohydrogenation of Nitrogen to Ammonia

Shang

Song

et al. 2022

CCS Chem

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“…Therefore, SACs have played a vital role in a myriad of key electrocatalytic reactions, including but not limited to, ORR, CO 2 RR, and NRR. [145][146][147][148][149][150] In addition, the gap between heterogenous and homogenous catalysis is expected to be bridged with the aid of SACs. [151] Latest years have witnessed the application of SACs in advanced rechargeable battery system owing to their numerous merits, encompassing maximum atom utilization, unsaturated coordination architecture, unique electrochemical property, and optimal electronic structure.…”

Section: Single Atommentioning

confidence: 99%

Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives

Shi

Sun

et al. 2021

Advanced Energy Materials

157

141

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as well as the cost-effectiveness and environmental-friendliness of sulfur resource. [1][2][3][4][5][6][7][8] However, a suite of troublesome problems, mainly pertaining to sluggish redox kinetics and severe polysulfide (PS) shuttle, has hampered the pathway for pursuing Li-S commercialization. [9][10][11][12][13] For one thing, the conversion from PS to Li 2 S exhibits large energy barriers, which is regarded as the rate-determining step of sulfur reduction reaction (SRR) process. For another, Li 2 S is prone to accumulating at the cathode side, which is not easy to be efficiently dissociated.Recent years have witnessed a burgeoning interest in designing adsorptive and electrocatalytic mediators for effective PS management in Li-S realm, in order to essentially expedite redox kinetics and inhibit "shuttle effect." [14][15][16][17][18][19][20] Although strenuous efforts have been devoted to exploring various types of PS mediators including carbonaceous materials, [21][22][23][24][25] metal oxides/carbides/nitrides/borides/ sulfides/selenides/phosphides, [26][27][28][29][30][31][32][33][34][35][36] and heterostructures, [37][38][39][40][41][42][43][44] their unsatisfactory adsorptive and catalytic behavior caused by insufficient active sites remains a huge barrier for obtaining favorable Li-S chemistry. To circumvent this problem, adjusting the morphology of PS mediators such as reducing their size to nanoscale has been recognized as a promising method to expose more active lattice planes and edge sites. Indeed, a myriad of PS mediators possessing ultrafine nanoparticle and ultrathin nanosheet architecture has been developed to efficiently adsorb sulfur species and catalyze PS conversion. [45][46][47][48][49] Furthermore, optimizing the electronic structure of PS mediator also serves as an appealing approach to boost electrochemical activities. [50][51][52][53][54] Defect engineering, an essential strategy to tailor the atomic distribution and dictate the surface property of nanomaterials, [55][56][57][58][59][60] plays a pivotal role in optimizing the electronic structure and promoting the electrochemical performance of catalysts in various scenarios including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO 2 RR), and nitrogen reduction reaction (NRR). [61][62][63][64][65][66][67][68][69][70][71][72] Very recently, defect engineering has stimulated a growing attention on PS mediator design in Li-S realm. Benefiting from a collection of compelling functionalities, defective mediator showcases remarkable promise in regulating PS behavior and realizing fast redox chemistry, thereby paving an innovative way toward practical applications of Li-S batteries.Lithium-sulfur (Li-S) batteries have stimulated a burgeoning scientific and industrial interest owing to high energy density and low materials costs. The favorable reaction kinetics of sulfur species is a key prerequisite for pursuing their commercialization. Recent years have ...

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“…Also recently, atomically dispersed Mn single atoms on nitrogen doped carbon were produced from pyrolysis of a polypyrrole polymer produced via in situ polymerization with MnO 2 that served as a polymerization initiator of the pyrrole monomers, but also as a sacrificial template and metal source. The obtained materials were employed as photocatalyst in CO 2 reduction to produce synthesis gas [64].…”

Section: Pyrolysismentioning

confidence: 99%

Carbon-Based Materials for the Development of Highly Dispersed Metal Catalysts: Towards Highly Performant Catalysts for Fine Chemical Synthesis

et al. 2020

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Single-atom catalysts (SACs), consisting of metals atomically dispersed on a support, are considered as advanced materials bridging homogeneous and heterogeneous catalysis, representing the catalysis at the limit. The enhanced performance of these catalysts is due to the combination of distinct factors such as well-defined active sites, comprising metal single atoms in different coordination environments also varying its valence state and strongly interacting with the support, in this case porous carbons, maximizing then the metal efficiency in comparison with other metal surfaces consisting of metal clusters and/or metal nanoparticles. The purpose of this review is to summarize the most recent advances in terms of both synthetic strategies of producing porous carbon-derived SACs but also its application to green synthesis of highly valuable compounds, an area in which the homogeneous catalysts are classically used. Porous carbon-derived SACs emerge as a type of new and eco-friendly catalysts with great potential. Different types of carbon forms, such as multi-wall carbon nanotubes (MWCNTs), graphene and graphitic carbon nitride or even others porous carbons derived from Metal–Organic-Frameworks (MOFs) are recognized. Although it represents an area of expansion, experimentally and theoretically, much more future efforts are needed to explore them in green fine chemical synthesis.

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In-situ polymerization induced atomically dispersed manganese sites as cocatalyst for CO2 photoreduction into synthesis gas

Cited by 62 publications

References 33 publications

Atomically Dispersed Manganese Lewis Acid Sites Catalyze Electrohydrogenation of Nitrogen to Ammonia

Atomically Dispersed Manganese Lewis Acid Sites Catalyze Electrohydrogenation of Nitrogen to Ammonia

Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives

Carbon-Based Materials for the Development of Highly Dispersed Metal Catalysts: Towards Highly Performant Catalysts for Fine Chemical Synthesis

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