Water oxidation on a mononuclear manganese heterogeneous catalyst

Guan, Jingqi; Duan, Zhiyao; Zhang, Fuxiang; Kelly, Shelly D.; Si, Rui; Dupuis, Michel; Huang, Qinge; Chen, John Qianjun; Tang, Chunhua; Li, Can

doi:10.1038/s41929-018-0158-6

Cited by 268 publications

(216 citation statements)

References 71 publications

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“…Because S atoms are less electronegative than N atoms, the coordinated S atoms could reduce the electron donation of the Ni atom to its neighboring N atoms (Figure k), thereby optimizing the hybridization states between Ni and the neighboring N atoms, and resulting in enhanced OER activity. Likewise, MnN 4 sites embedded in a graphene plane (Mn‐NG) have been studied, showing an overpotential of 337 mV at a current density of 10 mA cm −2 in alkaline media . The Tafel slope of Mn‐NG (55 mV dec −1 ), which is close to precious metal catalysts, is far smaller than that of the N‐free control sample (139 mV dec −1 ), indicating faster reaction kinetics.…”

Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

293

240

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Carbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.

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Section: Atomically Dispersed Single Metal Site Electrocatalysis For mentioning

confidence: 99%

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Zhu

Sokolowski

Song

et al. 2019

Advanced Energy Materials

293

240

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“…Other methods There are also other methods for synthesizing WOCs. [14].Copyright:2018 Springer Nature. [15] The mass-selected soft-landing method can also be applied to synthesize WOCs.…”

Section: Chemical Reductiona Nd Oxidationmentioning

confidence: 99%

“…The two DFT structures exhibited in Figure 2b couldb ee asily interconverted under certain conditions, as demonstrated through DFT calculations. [53] Considering the high catalytic activitya nd stability,m ultinuclear Mn 12 DH [23] and mononuclear Mn-NG, [14] which exhibit excellent performances, have been synthesized.W OCs with low overpotential, high TOF (Table 1), and strong durability can bring some new insightsi nto the preparation of increasingly efficient catalysts for the OER. EPR spectroscopy can be used to monitor the catalytic process, and every Ss tate has itso wn EPR signal.…”

Section: Manganese-based Wocsmentioning

confidence: 99%

“…[7] Additionally,t here are other examples of efficient multinuclear WOCs for the first-row transition-metal (TM) complexes,s uch as some multinuclear cobalt polyoxometalates (POMs) [8] and tetranuclear copper complexes. Because mononuclear WOCs are easily prepared and the structure can be controllably synthesized, some mononuclear WOCs have been prepared recently,s uch as mononuclear manganese embedded in nitrogen-doped graphene (Mn-NG), [14] AgCu, [15] and Ni-PY5 (PY5:2 ,6-bis[1,1-bis(2-pyridyl)ethyl]pyridine). [10] On multinuclear catalysts, the formation of the OÀOb ond is usually regarded as the rate-determining step during the OER.…”

Section: Introductionmentioning

confidence: 99%

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Mono‐/Multinuclear Water Oxidation Catalysts

Zhang

Guan

2019

ChemSusChem

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Water splitting, in which water molecules can be transformed into hydrogen and oxygen, is an appealing energy conversion and transformation strategy to address the environmental and energy crisis. The oxygen evolution reaction (OER) is dynamically slow, which limits energy conversion efficiency during the water‐splitting process and requires high‐efficiency water oxidation catalysts (WOCs) to overcome the OER energy barrier. It is generally accepted that multinuclear WOCs possess superior OER performances, as demonstrated by the CaMn4O5 cluster in photosystem II (PSII), which can catalyze the OER efficiently with a very low overpotential. Inspired by the CaMn4O5 cluster in PSII, some multinuclear WOCs were synthesized that could catalyze water oxidation. In addition, some mononuclear molecular WOCs also show high water oxidation activity. However, it cannot be excluded that the high activity arises from the formation of dimeric species. Recently, some mononuclear heterogeneous WOCs showed a high water oxidation activity, which testified that mononuclear active sites with suitable coordination surroundings could also catalyze water oxidation efficiently. This Review focuses on recent progress in the development of mono‐/multinuclear homo‐ and heterogeneous catalysts for water oxidation. The active sites and possible catalytic mechanisms for water oxidation on the mono‐/multinuclear WOCs are provided.

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“…

Heterogeneous,m etal, single-site catalysts often exhibit higher catalytic performance than other catalysts because of their maximized atom efficiency of 100 %. [5][6][7] Dispersing metal active sites into isolated metal atoms (ions) is an effective strategy for solving these problems.T herefore,m any atomically dispersed catalysts with either single atoms or mononuclear metal complexes (single metal ions) have been prepared for this purpose. Pd@POP was easy to use in regioselective organic reactions because the internal structure of this Pd@POP can be easily modified.

…”

mentioning

confidence: 99%

Constructing Mononuclear Palladium Catalysts by Precoordination/Solvothermal Polymerization: Recyclable Catalyst for Regioselective Oxidative Heck Reactions

Xiong

et al. 2019

Angew Chem Int Ed

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Heterogeneous,m etal, single-site catalysts often exhibit higher catalytic performance than other catalysts because of their maximized atom efficiency of 100 %. Reported herein is aprecoordination/solvothermal polymerization strategy to fabricate as table mononuclear Pd-metalized porous organic polymer catalyst (Pd@POP). Pd@POP was easy to use in regioselective organic reactions because the internal structure of this Pd@POP can be easily modified. The catalyst was used to solve the intractable regioselectivity problems of Heck reactions.Pd@POP-9 can efficiently activate the ends of olefins,therebyleading to high selectivity for substitution at the external position. To understand the reason underlying the high selectivity and activity of the catalyst, the systemic characterization of Pd@POP-9 and density-functional theory calculations were conducted. This Heckr eaction is the first to be catalyzedb yarecyclable mononuclear metal catalyst with unprecedented catalytic activity and regioselectivity.Compared with the homogeneous metal/ligand catalytic mode,t he heterogenization of corresponding homogeneous catalysts is an attractive tool for achieving recyclable catalysts and highly selective organic synthesis. [1][2][3][4] Forh eterogeneous catalysts,decreasing the size of catalytic metals can maximize the utilization of precious metals.B ecause only as mall number of metal particles,with appropriate size distribution, can be used as catalytic active sites,and particles of other sizes are either inert or cause side reactions. [5][6][7] Dispersing metal active sites into isolated metal atoms (ions) is an effective strategy for solving these problems.T herefore,m any atomically dispersed catalysts with either single atoms or mononuclear metal complexes (single metal ions) have been prepared for this purpose. [8][9][10][11] Fora tomically dispersed catalysts,t he support is very important. [12] Unfortunately,i n the existing literature,m ost supports do not play the role of the ligand, thereby preventing its large-scale application in ligand-controlled regioselective organic reactions. [13] For metal-catalyzed organic reactions,l igands generally play as ignificant role.I ns ome organic reactions,t he costs of ligands are more expensive than those of the corresponding metal catalysts. [14,15] Therefore,t he development of ah ighly efficient ligand that can be recycled and applied as asupport to am ononuclear metal catalyst will result in the development of modern organic synthesis methods.Porous organic polymers (POPs) have remained aperennial focus as an intriguing platform for incorporating homogeneous metal/ligand catalytic systems into heterogeneous supports. [16][17][18][19] In our previous work, [20][21][22][23] we demonstrated the advantages of phosphorus-doped (P-doped) POPs in catalytic regioselective and chemoselective reactions,a nd as an effective metal support for as ingle-site catalyst. When Pdoped POPs are used as supports,m ononuclear metal catalysts with 100 %m etal dispersion can be efficiently synthe...

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Water oxidation on a mononuclear manganese heterogeneous catalyst

Cited by 268 publications

References 71 publications

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

Mono‐/Multinuclear Water Oxidation Catalysts

Constructing Mononuclear Palladium Catalysts by Precoordination/Solvothermal Polymerization: Recyclable Catalyst for Regioselective Oxidative Heck Reactions

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