A universal approach to dual-metal-atom catalytic sites confined in carbon dots for various target reactions.

Here, a molecular-design and carbon dot-confinement coupling strategy through the pyrolysis of bimetallic complex of diethylenetriamine pentaacetic acid under low-temperature is proposed as a universal approach to dual-metal-atom sites in carbon dots (DMASs-CDs). CDs as the "carbon islands" could block the migration of DMASs across "islands" to achieve dynamic stability. More than twenty DMASs-CDs with specific compositions of DMASs (pairwise combinations among Fe, Co, Ni, Mn, Zn, Cu, and Mo) have been synthesized successfully. Thereafter, high intrinsic activity is observed for the probe reaction of urea oxidation on NiMn-CDs. In situ and ex situ spectroscopic characterization and first-principle calculations unveil that the synergistic effect in NiMn-DMASs could stretch the urea molecule and weaken the N-H bond, endowing NiMn-CDs with a low energy barrier for urea dehydrogenation. Moreover, DMASs-CDs for various target electrochemical reactions, including but not limited to urea oxidation, are realized by optimizing the specific DMAS combination in CDs.

PtPd Atomic Layer Shelled PdCu Hollow Nanoparticles on Partially Unzipped Carbon Nanotubes for Breaking the Activity-Stability Trade-Off toward the Hydrogen Oxidation Reaction in Alkaline Media.

Developing highly active yet stable catalysts for the hydrogen oxidation reaction (HOR) in alkaline media remains a significant challenge. Herein, we designed a novel catalyst of atomic PtPd-layer shelled ultrasmall PdCu hollow nanoparticles (HPdCu NPs) on partially unzipped carbon nanotubes (PtPd@HPdCu/W-CNTs), which can achieve a high mass activity, 5 times that of the benchmark Pt/C, and show exceptional stability with negligible decay after 20,000 cycles of accelerated degradation test. The atomically thin PtPd shell serves as the primary active site for the HOR and a protective layer that prevents Cu leaching. Additionally, the HPdCu substrate not only tunes the adsorption properties of the PtPd layer but also prevents corrosive Pt from reaching the interface between NPs and the carbon support, thereby mitigating carbon corrosion. This work introduces a new strategy that leverages the distinct advantages of multiple components to address the challenges associated with slow kinetics and poor durability toward the HOR.

Advanced Nanocarbons Toward two-Electron Oxygen Electrode Reactions for H2O2 Production and Integrated Energy Conversion.

Hydrogen peroxide (H2O2) plays a pivotal role in advancing sustainable technologies due to its eco-friendly oxidizing capability. The electrochemical two-electron (2e-) oxygen reduction reaction and water oxidation reaction present an environmentally green method for H2O2 production. Over the past three years, significant progress is made in the field of carbon-based metal-free electrochemical catalysts (C-MFECs) for low-cost and efficient production of H2O2 (H2O2EP). This article offers a focused and comprehensive review of designing C-MFECs for H2O2EP, exploring the construction of dual-doping configurations, heteroatom-defect coupling sites, and strategic dopant positioning to enhance H2O2EP efficiency; innovative structural tuning that improves interfacial reactant concentration and promote the timely release of H2O2; modulation of electrolyte and electrode interfaces to support the 2e- pathways; and the application of C-MFECs in reactors and integrated energy systems. Finally, the current challenges and future directions in this burgeoning field are discussed.

Fe/Co dual metal catalysts modulated by S-ligands for efficient acidic oxygen reduction in PEMFC.

Here, we report a conceptual strategy for introducing spatial sulfur (S)-bridge ligands to regulate the coordination environment of Fe-Co-N dual-metal centers (Spa-S-Fe,Co/NC). Benefiting from the electronic modulation, Spa-S-Fe,Co/NC catalyst showed remarkably enhanced oxygen reduction reaction (ORR) performance with a half-wave potential (E1/2) of 0.846 V and satisfactory long-term durability in acidic electrolyte. Combined experimental and theoretical studies revealed that the excellent acidic ORR activity with a remarkable stability observed for Spa-S-Fe,Co/NC is attributable to the optimal adsorption-desorption of ORR oxygenated intermediates achieved through charge-modulation of Fe-Co-N bimetallic centers by the spatial S-bridge ligands. These findings provide a unique perspective to regulate the local coordination environment of catalysts with dual-metal-centers to optimize their electrocatalytic performance.

Tailoring the Atomic-Local Environment of Carbon Nanotube Tips for Selective H2 O2 Electrosynthesis at High Current Densities.

The atomic-local environment of catalytically active sites plays an important role in tuning the activity of carbon-based metal-free electrocatalysts (C-MFECs). However, the rational regulation of the environment is always impeded by synthetic limitations and insufficient understanding of the formation mechanism of the catalytic sites. Herein, the possible cleavage mechanism of carbon nanotubes (CNTs) through the crossing points during ball-milling is proposed, resulting in abundant CNT tips that are more susceptible to be modified by heteroatoms, achieving precise modulation of the atomic environment at the tips. The obtained CNTs with N,S-rich tips (N,S-TCNTs) exhibit a wide potential window of 0.59 V along with H2 O2 selectivity for over 90.0%. Even using air as the O2 source, the flow cell system with N,S-TCNTs catalyst attains high H2 O2 productivity up to 30.37 mol gcat. -1  h-1 @350 mA cm-2 , superior to most reported C-MFECs. From a practical point of view, a solid electrolyzer based on N,S-TCNTs is further employed to realize the in-situ continuous generation of pure H2 O2 solution with high productivity (up to 4.35 mmol cm-2  h-1 @300 mA cm-2 ; over 300 h). The CNTs with functionalized tips hold great promise for practical applications, even beyond H2 O2 generation.

[Effects of vegetation recovery practices on the characteristics of soil nematode communities on seriously degraded grasslands in Songnen Plain].

In this paper, the data of soil nematodes on the seriously degraded grasslands in Songnen Plain under different vegetation recovery practices were collected from May to October, 2005, and the community structure and its seasonal changes of the nematodes were studied by using the community parameters of generic richness, abundance, diversity index, and functional group index. The results showed that both fencing enclosure and planting Puccinellia chinampoensis could improve the nematode communities substantially. The nematode abundance and diversity were significantly higher in planting P. chinampoensis than in fencing enclosure, whereas the generic richness and evenness had no significant difference between these two vegetation recovery practices. The functional group index indicated that fencing enclosure and planting P. chinampoensis altered the ratio of rho- and kappa- choice of plant parasite nematodes. Compared with free-living nematodes, plant parasite nematodes were more sensitive to the vegetation recovery practices. On the seriously degraded grasslands in Songnen Plain, planting P. chinampoensis could be more favorable to the restoration of soil nematode communities than fencing enclosure.