Chemical Reviews最新文献

Optical imaging through scattering media is important in a variety of fields ranging from microscopy to autonomous vehicles. Although advanced wavefront shaping techniques have offered several breakthroughs in the past decade, current techniques still require a known guide star and a high-resolution spatial light modulator or a very large number of measurements and are limited in their correction field of view. Here we introduce a guide-star-free, non-invasive approach that can correct more than 190,000 scattered modes using only 25 incoherently compounded, holographically measured, scattered light fields, obtained under unknown random illuminations. This is achieved by computationally emulating an image-guided wavefront shaping experiment, where several virtual spatial light modulators are simultaneously optimized to maximize the reconstructed image quality. Our method shifts the burden from the physical hardware to a digital, naturally parallelizable computational optimization, leveraging state-of-the-art automatic differentiation tools. We demonstrate the flexibility and generality of this framework by applying it to imaging through various complex samples and imaging modalities, including epi-illumination, anisoplanatic multi-conjugate correction of highly scattering layers, lensless endoscopy in multicore fibres and acousto-optic tomography. The presented approach offers high versatility, effectiveness and generality for fast, non-invasive imaging in diverse applications.

High-performance thermoelectric materials at room temperature are eagerly pursued due to their promising applications in the Internet of Things for sustainable power supply. Reducing sound velocity by softening chemical bonds is considered an effective approach to lowering thermal conductivity and enhancing thermoelectric performance. Here, different from softening chemical bonds at the atomic scale, we introduce a global softening strategy, which macroscopically softens the overall material to manipulate its sound velocity. This is demonstrated in MgAgSb, one of the most promising p-type thermoelectric materials at room temperature to replace (Bi,Sb)₂Te₃, that the addition of inherently soft organic compounds can easily lower its sound velocity, leading to an obvious reduction in lattice thermal conductivity. Despite a simultaneous reduction of the power factor, the overall thermoelectric quality factor B is enhanced, enabling softened MgAgSb by C₁₈H₃₆O₂ addition to achieve a figure of merit zT value of ∼0.88 at 300 K and a peak zT value of ∼1.30. Consequently, an impressive average zT of ∼1.17 over a wide temperature range has been realized. Moreover, this high-performance MgAgSb is verified to be highly repeatable and stable. With this MgAgSb, a decent conversion efficiency of 8.6% for a single thermoelectric leg and ∼7% for a two-pair module have been achieved under a temperature difference of ∼276 K, indicating its great potential for low-grade heat harvesting. This work will not only advance MgAgSb for low-grade power generation, but also inspire the development of high-performance thermoelectrics with global softening in the future.

Underutilized wastewaters containing dilute levels of reactive nitrogen (Nr) can help rebalance the nitrogen cycle. This study describes electrodialysis and nitrate reduction (EDNR), a reactive electrochemical separation architecture that combines catalysis and separations to remediate nitrate and ammonium-polluted wastewaters while recovering ammonia. By engineering operating parameters (e.g., background electrolyte, applied potential, electrolyte flow rate), we achieved high recovery and conversion of Nr in both simulated and real wastewaters. The EDNR process demonstrated long-term robustness and up-concentration that recovered >100 mM ammonium fertilizer solution from agricultural runoff that contained 8.2 mM Nr. EDNR is the first reported process to our knowledge that remediates dilute real wastewater and recovers ammonia from multiple Nr pollutants, with an energy consumption (245 MJ per kg NH₃–N in simulated wastewater, 920 MJ per kg NH₃–N in agricultural runoff) on par with the state-of-the-art. Demonstrated first at proof-of-concept and engineered to technology readiness level (TRL) 4–5, EDNR shows great promise for distributed wastewater treatment and sustainable ammonia manufacturing.

While a rapid defossilisation of the energy-industry system is at the highest priority for climate change mitigation, additional post-fossil carbon dioxide removal (CDR) for net-negative emissions will likely be necessary to ensure a safe future. An in-depth techno-economic analysis of differentiated sequestration options for carbon dioxide (CO₂) in solid carbonates is not yet available, as direct air capture-based mineralisation is usually aggregated in direct air capture and carbon sequestration. This research gap is closed by studying mineralisation as a key CDR option to sequester atmospheric CO₂ permanently, based on available literature. The most frequently discussed routes for mineralisation, i.e., in situ, ex situ mineralisation, and enhanced rock weathering, are examined. The deployment potentials of these options are determined globally for nine major regions. Results indicate that costs for all mineralisation options can be kept below 100 € per tCO₂ from 2050. From 2030 onwards, in situ mineralisation, with low energy-intensity, can be realised at cost of ≤131 € per tCO₂, ex situ mineralisation at ≤189 € per tCO₂, and enhanced weathering at ≤88 € per tCO₂. Final energy demand for CO₂ sequestration via in situ mineralisation is ≤1.8 MWh per tCO₂, via ex situ mineralisation ≤3.7 MWh per tCO₂, and via enhanced weathering ≤1.1 MWh per tCO₂ from 2030. Large-scale deployment of mineralisation options supporting 60% of projected CDR demand is assessed to require up to 0.06% and 0.21% in global gross domestic product and up to 2.5% and 8.6% additional primary energy demand in 2070 for a 1.5 °C and 1.0 °C climate target, respectively. Implications, permanence of sequestration, and limitations are discussed, and a research outlook is provided.